WO2013018356A1

WO2013018356A1 - Method for producing composite particle, method for producing cosmetic, and cosmetic

Info

Publication number: WO2013018356A1
Application number: PCT/JP2012/004858
Authority: WO
Inventors: Yoshinori Inokuchi; Ryuichi Inaba
Original assignee: Shin Etsu Chemical Co Ltd
Current assignee: Shin Etsu Chemical Co Ltd
Priority date: 2011-08-04
Filing date: 2012-07-31
Publication date: 2013-02-07
Anticipated expiration: 2014-02-04
Also published as: TW201318640A

Abstract

The present invention provides a method for producing a composite particle, wherein a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into a mixed solution obtained by blending, at least, a mixed aqueous disperse solution in which an inorganic powder and a silicone elastomer are dispersed, a cationic water-soluble polymer, and an alkaline substance, whereby carrying out a hydrolysis-condensation reaction to produce a composite particle formed of the inorganic powder whose surface is adhered with the silicone elastomer by using a silicone resin as a binder. There can be provided a method for producing, regardless of the kind of inorganic powders, a composite particle in which a silicone elastomer is adhered uniformly onto surface of an inorganic powder.

Description

METHOD FOR PRODUCING COMPOSITE PARTICLE, METHOD FOR PRODUCING COSMETIC, AND COSMETIC

The present invention relates to a method for producing a composite particle, specifically a method for producing a composite particle having a silicone elastomer adhered onto surface of an inorganic powder; a method for producing a cosmetic using the composite particle which is produced by the method for producing the composite particle; and a cosmetic.

Makeup cosmetics such as foundation is used to conceal configuration troubles such as skin wrinkles, pores, and texture roughness, or skin tone troubles such as blemishes and freckles thereby giving a smooth and beautiful skin look; and in recent years makeup with a non-artificial, natural finish feeling (bare skin feeling) is considered to be important. In addition, makeup with a natural finish feeling of cosmetics is given a high value when it has no artificial gloss (shiny) but has excellent evenness in cosmetic coating and high transparency.

In the past, many new materials and new technologies have been proposed to obtain a natural makeup feeling while maintaining the foregoing effects in a makeup cosmetic. Especially, to conceal a figure trouble, cosmetics which are blended with various kinds of powders of a diffusion-reflection type have been known. In PTL 1, a multilayer cosmetic to conceal wrinkles, formed of a combination of a makeup foundation for a first layer containing an adhesive material and a makeup finishing material for a second layer containing a powder which diffuse-reflects a light, has been proposed. In this multilayer cosmetic to conceal wrinkles, for example, a composite powder of a light diffusion-reflection type having a talc particle covered with an acryl type polymer is used.

In this cosmetic, however, there has been a drawback that, when a cosmetic film is kept on a skin for a long period of time, a sebum is mixed with an adhesive material thereby causing deviation from a proper mixing range of the powder with the adhesive material, this in turn leading to decrease in effects of the cosmetic. In PTL 2, a flake-like micropowder having surface of a flake-like material such as a natural mica covered with a spherical silica microparticle is disclosed. It is mentioned, because this flake-like micropowder uses a spherical microparticle having a large surface diffusion scattering effect of a light, when this flake-like micropowder is used as a cosmetic ingredient, a technical effect, quoted as saying, "An excessive gloss of a substrate mica can be suppressed, and at the same time a so-called soft focus effect such as to make a small wrinkle unnoticeable can be expressed. In addition, a cosmetic having further improved properties such as a sliding property and a feeling during the time of its use can be obtained." can be expressed.

However, because the flake-like micropowder has an extraordinarily good sliding property, a cosmetic blended with this is prone to form irregularity during the time of its application whereby uniform application of this cosmetic is difficult; and thus, there is a drawback that a natural makeup feeling cannot be obtained. In addition, a silica microparticle used as a covering material decreases a contact area between the composite powder and a skin thereby decreasing adhesion thereof with a skin, and this in turn making the composite powder readily removed from a skin by a physical impact such as scuffing by a cloth; and thus, there is a drawback that durability of a cosmetic effect is decreased. If the ratio of the silica microparticle in the flake-like micropowder is reduced with an aim to enhance adhesion of the composite powder to a skin, there is a drawback that an effect to a figure trouble cannot be adequately obtained.

There have been known more technologies similar to those of the above-mentioned to avoid a figure trouble or to perform a natural makeup feeling; such as for example, a cosmetic which contains a pigment having a core-shell structure wherein a core of a flake-like pigment is covered with a colored pigment-containing titanium dioxide and then on it with a light-diffusing powder (PTL 3); a technology to blend a cosmetic with a composite powder having surface of a clay mineral covered with an inorganic metal hydroxide such as aluminum hydroxide (PTL 4 and PTL 5); a cosmetic which contains a powder having surface of a powder - having refractive index of 1.6 to 1.7 such as barium sulfate - covered with a layer of a metal oxide having a high refractive index and then on it with a layer of one, or two or more materials selected from yellow iron oxide, black iron oxide, and red iron oxide (PTL 6); and a cosmetic which contains a silica-zinc oxide composite obtained from a silica sol, zinc oxide, and so on (PTL 7).

However, although these composite powders express a soft focus effect to some extent by their light-diffusion effects, in view of a use feeling of a cosmetic, satisfactory effects in softness, moistness, smoothness, and the like cannot be obtained because of hardness of the composite powders themselves which are formed of an inorganic metal oxide or an inorganic metal hydroxide. On the other hand, to improve a use feeling of a cosmetic powder, namely in order to afford thereto a use feeling such as non-stickiness and smoothness, a spreading property, and an adhesion property, a proposal is made in PTL 8 on the particle having surface of a scale-like inorganic particle covered with a polyurethane, a styrene-butadien copolymer, a silicone elastomer, or a polyolefin elastomer; it is mentioned therein that a soft and moist feeling can be obtained.

However, a specific example of the particle covered with a silicone elastomer has not been mentioned. In other literatures, a particle whose surface is adhered and covered with a silicone elastomer and a method for producing it have been proposed. In PTL 9, a method for crushing and mixing a silica and a silicone elastomer having a reactive functional group is proposed; but a particle which maintains initial particle form and size cannot be obtained because a silica particle, which is a mother particle, is crushed. In other words, it has drawbacks that a particle having a certain form such as a spherical, a plate-like, and a rod-like form cannot be obtained and a diameter thereof cannot be controlled. In PTL 10, a method wherein a mother particle and a curable silicone which becomes a silicone elastomer is mixed, and then the silicone is cured is proposed; but a plurality of mother particles are contained in the particle thus obtained. In PTL 11, a method wherein a mixture of a silica particle which becomes a mother particle and a curable silicone which becomes a silicone elastomer is emulsified and dispersed in water, and then the silicone is cured is proposed; and in PTL 12, a method wherein a mixture of an aqueous dispersion of silica particles and a curable silicone which becomes a silicone elastomer is emulsified and dispersed in water, and then the silicone is cured is proposed. In these methods, however, a particle containing a plurality of the mother particles or a particle not containing the mother particle is formed occasionally.

In view of the above, inventors of the present invention made a proposal in PTL 13 on a composite particle wherein into an aqueous mixed disperse solution of a powder and a silicone elastomer is added an acidic substance or an alkaline substance and a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them whereby performing a hydrolysis-condensation reaction of this compound to adhere the silicone elastomer having a light diffusion property onto surface of an arbitrary nuclear powder by using a silicone resin as a binder; a cosmetic blended with this can visually express a corrective effect of a skin figure trouble and can be provided with a use feeling of non-stickiness, softness, and moistness - which are coherent characteristics of the silicone elastomer -, with good properties in spreading, softness, adhesion, and mixing, and with a corrective effect of a skin figure.

[PTL 1] Japanese Patent Laid-Open Publication No. H06-128122
[PTL 2] International Patent Laid-Open Publication No. 92/03119
[PTL 3] Japanese Patent Laid-Open Publication No. H08-188723
[PTL 4] Japanese Patent Laid-Open Publication No. H09-20609
[PTL 5] Japanese Patent Laid-Open Publication No. 2002-146238
[PTL 6] Japanese Patent Laid-Open Publication No. 2003-40737
[PTL 7] Japanese Patent No. 3702072
[PTL 8] Japanese Patent No. 3963635
[PTL 9] Japanese Patent Laid-Open Publication No. H08-3451
[PTL 10] Japanese Patent Laid-Open Publication No. H03-294357
[PTL 11] Japanese Patent Laid-Open Publication No. H02-232263
[PTL 12] Japanese Patent Laid-Open Publication No. H03-281536
[PTL 13] Japanese Patent Laid-Open Publication No. 2011-1332

However, in the case that a nuclear powder is an inorganic powder, depending on the kind thereof, there have been problems that a silicone elastomer particle does not adhere thereonto, adhesion thereof is uneven, and a providing effect of the forgoing properties to a cosmetic is insufficient.

The present invention was made in view of the situation mentioned above, and thus has an object to provide; a method for producing a composite particle which can adhere a silicone elastomer onto surface of an inorganic powder regardless of kind of the powders; and a cosmetic having good spreading, softness, adhesion, and mixing properties.

To solve the problems mentioned above, the present invention provides a method for producing a composite particle, wherein a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into a mixed solution obtained by blending, at least, a mixed aqueous disperse solution in which an inorganic powder and a silicone elastomer are dispersed, a cationic water-soluble polymer, and an alkaline substance, whereby carrying out a hydrolysis-condensation reaction to produce a composite particle formed of the inorganic powder whose surface is adhered with the silicone elastomer by using a silicone resin as a binder.

According to the method as mentioned above, a composite particle in which a silicone elastomer is adhered uniformly onto surface of an inorganic powder can be obtained regardless of the kind of the inorganic powder.

It is preferable that the cationic water-soluble polymer is synthetic, not containing an anionic and an amphoteric group, obtained by synthesizing a polymer skeleton thereof with any of a vinyl polymerization, an addition polymerization, and a condensation.
If the cationic water-soluble polymer as mentioned above is used, the said polymer assists adsorption of the silicone elastomer onto the inorganic powder so that the silicone elastomer can be uniformly adhered onto surface of the inorganic powder without agglomeration of the silicone elastomer.

In addition, it is preferable that the cationic water-soluble polymer synthesized without using a monomer having a nonionic group is used.
The cationic water-soluble polymer synthesized without using a monomer having a nonionic group can make the silicone elastomer adhered on surface of the inorganic powder more uniformly.

In addition, it is preferable that a polymer of dimethyl diallyl ammonium chloride is used as the cationic water-soluble polymer.
The polymer of dimethyl diallyl ammonium chloride can make the silicone elastomer adhered on surface of the inorganic powder more uniformly.

In addition, adding amount of the cationic water-soluble polymer to the mixed aqueous disperse solution is preferably in the range of 0.0001 to 1 part by mass relative to 100 parts by mass of water in the mixed aqueous disperse solution.
Adding amount in the range as mentioned above can make the silicone elastomer adhered on surface of the inorganic powder more uniformly and can give a better adhesion state.

In addition, the present invention provides a method for producing a cosmetic, wherein the cosmetic is produced by using the composite particle produced by the method for producing a composite particle.

According to the production method as mentioned above, a cosmetic with good spreading, softness, adhesion, and mixing properties, with an excellent corrective effect in a skin figure when it is used as a makeup cosmetic such as foundation, and with a good use feeling such as smoothness and non-stickiness can be produced.

Furthermore, the present invention provides a cosmetic, wherein the cosmetic contains a composite particle produced by a hydrolysis-condensation reaction of a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them added into a mixed solution containing a cationic water-soluble polymer, an alkaline substance, and an aqueous mixture disperse solution in which an inorganic powder and a silicone elastomer are dispersed, thereby forming the composite particle having the silicone elastomer adhered onto surface of the inorganic powder by using a silicone resin as a binder.

A cosmetic of the present invention as mentioned above has good spreading, softness, adhesion, and mixing properties with an excellent corrective effect in a skin figure.

In addition, it is preferable that the composite particle is produced by using the cationic water-soluble polymer which is a synthetic polymer whose polymer skeleton, containing neither an anionic group nor an amphoteric group, is synthesized by any of a vinyl polymerization, an addition polymerization, and a condensation.

A cosmetic containing the composite particle as mentioned above is provided with a good use feeling such as smoothness and non-stickiness.

In addition, it is preferable that the composite particle is produced by using the cationic water-soluble polymer which is synthesized by not using a monomer having a nonionic group.
A cosmetic which contains the composite particle as mentioned above is provided with further improved various properties as a cosmetic.

Further, it is preferable that the composite particle is produced by using a polymer of dimethyl diallyl ammonium chloride as the cationic water-soluble polymer.
A cosmetic which contains the composite particle as mentioned above is provided with further improved various properties as a cosmetic.

In addition, it is preferable that the composite particle is produced by using the cationic water-soluble polymer with the amount thereof against the aqueous mixture disperse solution being in the range of 0.0001 to 1 parts by mass relative to 100 parts by mass of water in the aqueous mixture disperse solution.

If the blending amount as mentioned above is used, adhesion of a silicone elastomer onto surface of an inorganic powder can be made more uniform and adhesion itself can be made better; and thus, a cosmetic is provided especially with good spreading, softness, adhesion, and mixing properties and with a more excellent corrective effect in a skin figure.

As mentioned above, according to the method for producing a composite particle of the present invention, a composite particle having a silicone elastomer evenly adhered onto surface of an inorganic powder regardless of kind of the inorganic particles can be obtained.
In addition, a composite particle like this which is produced by the method of the present invention is excellent in spreading, usability, adhesion, dispersion, figure corrective effect, water-resistance, and sebum-resistance; and thus, if a cosmetic is produced by using this particle, a cosmetic having good spreading, softness, adhesion, and mixing properties with an excellent figure corrective effect can be provided.
Further, a cosmetic of the present invention using the composite particle as mentioned above has a light and wide spreading property, so that it can be spread widely, softly, and evenly, and also has excellent dispersibility, sebum-resistance, and cosmetic durability; in addition, when this particle is blended into any kind of cosmetics, a cosmetic having excellent stability to temperature change and time passage can be obtained.

Fig. 1 is an electron micrograph of composite particles obtained in Example 1. Fig. 2 is an electron micrograph of composite particles obtained in Comparative Example 1.

Mode(s) for Carrying out the Invention

Hereinafter, the present invention will be explained in more detail.
As mentioned above, according to conventional methods for producing a composite particle, in the case that a nuclear powder is an inorganic powder, depending on the kind of the inorganic powder there has been a problem that a silicone elastomer particle is not adhered thereonto or its adhesion is uneven; and when the composite particle like this is used in a cosmetic, there has been a problem of an insufficient providing effect of the foregoing properties (such as spreading, softness, adhesion, and mixing properties and a corrective effect of a skin figure) to a cosmetic.

Inventors of the present invention carried out an extensive investigation to solve the problems as mentioned above, and as a result, the inventors found that, in a method to produce a composite particle wherein into an aqueous mixed disperse solution in which an inorganic powder and a silicone elastomer were dispersed were added an alkaline substance and a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them whereby performing a hydrolysis-condensation reaction of this compound, if a cationic water-soluble polymer was added into the aqueous mixed disperse solution, a composite particle having the silicone elastomer uniformly adhered onto surface of the inorganic powder, regardless of kind of the inorganic powders, by using a silicone resin as a binder; and in addition, the inventors found that a cosmetic blended with this composite particle could visually express a corrective effect of a skin figure trouble and could have a use feeling of non-stickiness, softness, and moistness, which are coherent characteristics of the silicone elastomer, while expressing good properties in spreading, softness, adhesion, and mixing, and a corrective effect of a skin figure. Based on these findings, the present invention could be accomplished.

Hereinafter, the present invention will be explained in the order of (I) a method for producing a composite particle, (II) a method for producing a cosmetic by using the composite particle, and (III) a cosmetic which contains the composite particle.

I. A method for producing a composite particle
A method for producing a composite particle of the present invention, wherein a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into a mixed solution obtained by blending, at least, a mixed aqueous disperse solution in which an inorganic powder and a silicone elastomer are dispersed, a cationic water-soluble polymer, and an alkaline substance, whereby carrying out a hydrolysis-condensation reaction to produce a composite particle formed of the inorganic powder whose surface is adhered with the silicone elastomer by using a silicone resin as a binder.

Here, in the present invention, "adhesion" of a silicone elastomer by using a silicone resin as a binder is preferably in a state that surface of an inorganic powder is adhered and covered by the silicone elastomer with a uniform thickness and without having a space; but, it is not restricted to this state, and thus, for example, a state that surface of the inorganic powder is adhered uniformly with having a space may be allowed.

<Inorganic powder>
As the inorganic powder used in the present invention, a powder substantially usable in a cosmetic with any range of particle diameter can be used. In addition, any geometric configuration including a spherical, a polyhedral, a spindle-shaped, a needle-like, and a plate-like configuration may be used provided that those configurations are used in a cosmetic; and in addition, the powder may be porous or non-porous.

The average particle diameter thereof is preferably in the range of 0.5 to 50 um, or more preferably 1 to 30 um. If the particle diameter is 0.5 um or more, a use feeling such as non-stickiness and smoothness or a providing effect of a spreading property does not decrease; or if the particle diameter is 50 um or less, a harsh feeling is not felt. Meanwhile, the average particle diameter can be measured by selecting an appropriate method from any of a microscopic method, a light-scattering method, a laser diffraction method, a liquid sedimentation method, an electric resistance method, and so on, in accordance with particle's morphology.

Illustrative examples of the inorganic powder include a particle of titanium oxide, titanium mica, zirconium oxide, zinc oxide, cerium oxide, magnesium oxide, barium sulfate, calcium sulfate, magnesium sulfate, calcium carbonate, magnesium carbonate, talc, cleaved talc, mica, kaolin, sericite, white mica, synthetic mica, golden mica, red mica, black mica, lithia mica, silicic acid, silicon dioxide, hydrated silicon dioxide, aluminum silicate, magnesium silicate, aluminum magnesium silicate, calcium silicate, barium silicate, strontium silicate, a metal tungstate, hydroxy apatite, vermiculite, haidilite, bentonite, montomorillonite, hectorite, zeolite, ceramics, dibasic calcium phosphate, alumina, aluminum hydroxide, boron nitride, and glass.

In addition, inorganic pigments may be mentioned. Specific examples thereof include an inorganic red pigment such as iron oxide, iron hydroxide, and iron titanate; an inorganic brown pigment such as gamma-iron oxide; an inorganic yellow pigment such as yellow iron oxide and yellow ocher; an inorganic black pigment such as black iron oxide and carbon black; an inorganic purple pigment such as manganese violet and cobalt violet; an inorganic green pigment such as chromium hydroxide, chromium oxide, cobalt oxide, and cobalt titanate; an inorganic blue pigment such as prussian blue and ultramarine; a colored pigment such as laked tar dye and laked natural dye; and a pearl pigment such as mica coated with titanium oxide, bismuth oxychloride, bismuth oxychloride coated with titanium oxide, talc coated with titanium oxide, argentine, and colored mica coated with titanium oxide.

In addition, illustrative examples of the inorganic particle include a metal microparticle of aluminum, copper, stainless steel, silver, and so on.

Meanwhile, if a light-interference powder such as mica titanium is selected as the inorganic powder of the present invention with the aim to express, among corrective effects of a skin figure, a three-dimensional make effect, i.e., especially to have a brighter and higher appearance in the T-zone from a forehead to a nose line or to suppress reflection of a light in the U-zone from a cheek to a chin thereby expressing an optical corrective effect so as to make a sagging skin unnoticeable, a light-interference powder of any one of a red type whose interference light has a reflection peak in the range of 550 to 700 nm and a blue type having a reflection peak in the range of 400 to 500 nm or both is especially preferable.

The foregoing inorganic powders may be surface-treated with a metal soap, a silane, a silicone, a silicone resin, a fluorine compound, an amino acid, an iron oxide, a titanium oxide, an iron oxide titanium oxide, or an aluminum hydroxide.

<Silicone elastomer>
The silicone elastomer used in the present invention may be produced, for example, by a method involving emulsification of a curable liquid silicone composition as described later; and thus, morphology thereof is spherical in many cases. Depending on reaction conditions, the effects thereof may not be significantly damaged in any of near sphere or partial agglomerate particle. In view of effectively expressing a use feeling of the silicone elastomer, the particle diameter thereof is preferably smaller than that of the foregoing inorganic powder to which the silicone elastomer is adhered. If the particle diameter thereof is smaller than that of the inorganic powder, a use feeling such as non-stickiness and smoothness of the powder and characteristics such as spreading and adhesion properties may be expressed more eminently. Smallness in the particle diameter thereof is not particularly restricted; and for example, in the case that the elastomer is produced by a method involving emulsification of a curable liquid silicone, the minimum particle diameter obtained by this method becomes the lower limit thereof.

The silicone elastomer is a rubber elastic body having a linear organosiloxane block shown by the following formula (1),
-(R¹ ₂SiO_2/2)_n- (1)
wherein R¹ represents a substituted or an unsubstituted monovalent hydrocarbon group having 1 to 30 carbon atoms, and "n" represents a positive number ranging from 5 to 5000.

Illustrative examples of R¹ include an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, a nonyl group, a decyl group, an undecyl group, a dodecyl group, a tetradecyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, an eicosyl group, a henicosyl group, a docosyl group, a tricosyl group, a tetracyl group, and a triacotyl group; a cycloalkyl group such as a cyclobutyl group, a cyclopentyl group, a cyclohexyl group, and a cycloheptyl group; an aryl group such as a phenyl group, a tolyl group, and a naphthyl group; an aralkyl group such as a benzyl group, a phenethyl group, and a beta-phenylpropyl group; an alkenyl group such as a vinyl group and an allyl group; and a hydrocarbon group whose part or all of hydrogen atoms bonded to a carbon atom of these groups is substituted with an atom such as a halogen atom (fluorine atom, chlorine atom, bromine atom, and iodine atom) and/or a substituent group, while illustrative examples of the said substituent group include an acryloyloxy group, a methacryloyloxy group, an epoxy group, a glycidoxy group, an amino group, a mercapto group, and a carboxyl group.

Rubber hardness of the silicone elastomer in its soft side is preferably 10 or more as measured by the E-type durometer, and preferably 90 or less in its hard side as measured by the A-type durometer, in accordance with JIS K 6253. More preferable hardness is 20 or more by the E-type durometer and 80 or less by the A-type durometer. If the hardness is 10 or more by the E-type durometer, agglomeration tendency is not so high that a use feeling such as non-stickiness and smoothness and a spreading property can be kept in a good condition. When the hardness is 90 or less by the A-type durometer, a soft feeling is not insufficient.

The silicone elastomer may be allowed sticky unless a use feeling such as non-stickiness and smoothness or a spreading property is decreased significantly. The silicone elastomer may contain in its particle a component such as a silicone oil, an organosilane, a silicone resin, an inorganic particle, an organic particle, and a liquid hydrocarbon oil, provided that they are approved in a cosmetic.

The silicone elastomer is obtained from a curable liquid silicone composition.
Illustrative examples of the curing reaction thereof include condensation reactions between a methoxy silyl group (SiOCH₃) and a hydroxy silyl group (SiOH), between a hydrosilyl group (SiH) and a hydroxy silyl group (SiOH), and so on; a radical reaction between a mercaptopropyl silyl group (Si-C₃H₆SH) and a vinyl silyl group (SiCH=CH₂); and an addition reaction between a vinyl silyl group (SiCH=CH₂) and a hydrosilyl group (SiH); however, in view of reactivity, a condensation reaction or an addition reaction is preferable.

For example, if the silicone elastomer is obtained by curing with the addition reaction, a curable liquid silicone composition comprising an organopolysiloxane shown by the following average composition formula (2) and containing at least 2 monovalent olefinic unsaturated groups in a molecule and an organohydrogen polysiloxane shown by the following average composition formula (3) and containing at least 3 silicon-bonded hydrogen atoms in a molecule may be subjected to the addition polymerization in the presence of a platinum-based catalyst with the blending ratio of the hydrosilyl group to the monovalent olefinic unsaturated group contained therein being 0.5 to 2.
R² _aR³ _bSiO_(4-a-b)/2 (2)
R⁴ _cH_dSiO_(4-c-d)/2 (3)

Here, in the average composition formula (2), R² represents a substituted or an unsubstituted monovalent hydrocarbon group having 1 to 30 carbon atoms except for aliphatic unsaturated group, and R³ represents monovalent olefinic unsaturated group having 2 to 6 carbon atoms. "a" and "b" represent positive numbers satisfying that "a" is 0 or more and less than 3, "b" is more than 0 and 3 or less, and a+b are 0.1 or more and 3 or less, preferably "a" is 0 or more and 2.295 or less, "b" is 0.005 or more and 2.3 or less, and a+b are 0.5 or more and 2.3 or less.

In the average composition formula (3), R⁴ represents a substituted or an unsubstituted monovalent hydrocarbon group having 1 to 30 carbon atoms except for aliphatic unsaturated group. "c" and "d" represent positive numbers satisfying that "c" is 0 or more and less than 3, "d" is more than 0 and 3 or less, and c+d are 0.1 or more and 3 or less, preferably "c" is 0 or more and 2.295 or less, "d" is 0.005 or more and 2.3 or less, and c+d are 0.5 or more and 2.3 or less.

Illustrative examples of R² include an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, a nonyl group, a decyl group, an undecyl group, a dodecyl group, a tetradecyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, an eicosyl group, a henicosyl group, a docosyl group, a tricosyl group, a tetracyl group, and a triacotyl group; a cycloalkyl group such as a cyclobutyl group, a cyclopentyl group, a cyclohexyl group, and a cycloheptyl group; an aryl group such as a phenyl group, a tolyl group, and a naphthyl group; an aralkyl group such as a benzyl group, a phenethyl group, and a beta-phenylpropyl group; and a hydrocarbon group whose part or all of hydrogen atoms bonded to a carbon atom of these groups is substituted with an atom such as a halogen atom (fluorine atom, chlorine atom, bromine atom, and iodine atom) and/or a substituent group, while illustrative examples of the said substituent group include an acryloyloxy group, a methacryloyloxy group, an epoxy group, a glycidoxy group, and a carboxyl group. A nonreactive group such as an alkyl group, an aryl group, an aralkyl group, and a cycloalkyl group is contained in R² with the amount thereof being preferably 80% or more by mole, or more preferably 90% or more by mole.

Illustrative examples of R³ include a vinyl group, an allyl group, a butenyl group, a pentenyl group, and hexenyl group, but a vinyl group is preferable industrially. Illustrative examples of R⁴ include the groups similar to R².

In order to obtain a particle having a smaller particle diameter efficiently by the method described later, dynamic viscosities of the organopolysiloxane containing olefinic unsaturated groups and the organohydrogen polysiloxane at 25 degrees C are preferably 1,000,000 mm²/second or less, or more preferably 500,000 mm²/second or less.
Meanwhile, these dynamic viscosities are measured by a capillary viscometer.

The organopolysiloxane containing olefinic unsaturated groups and the organohydrogen polysiloxane may be of any of a linear, a cyclic, and a branched structure.

Illustrative examples of the platinum-based catalyst include a single body of a metal belonging to the platinum group such as platinum (including platinum black), rhodium, and palladium; a platinum chloride, a chloroplatinic acid, and a chloroplatinate, such as H₂PtCl₄-kH₂O, H₂PtCl₆-kH₂O, NaHPtCl₆-kH₂O, KHPtCl₆-kH₂O, Na₂PtCl₆-kH₂O, K₂PtCl₄-kH₂O, PtCl₄-kH₂O, PtCl₂, and Na₂HPtCl₄-kH₂O (in these formulae, "k" represents an integer of 0 to 6, or preferably 0 or 6); an alcohol-modified chloroplatinic acid (US Patent No. 3220972); a complex of chloroplatinic acid with an olefin (US Patent No. 3159601, US Patent No. 3159662, and US Patent No. 3775452); a metal belonging to the platinum group, such as black platinum and palladium, with these metals being supported on a carrier such as alumina, silica, and carbon; a rhodium-olefin complex; chlorotris(triphenylphosphine) rhodium (Wilkinson catalyst); and a complex of platinum chloride, chloroplatinic acid, or chloroplatinic acid salt with a vinyl-containing siloxane, in particular a complex with a vinyl-containing siloxane.

For example, in the case of producing the silicone elastomer by curing with a condensation reaction, the elastomer may be produced by a polycondensation reaction of a liquid silicone composition comprising an organopolysiloxane having at least 2 silicon-bonded hydroxyl groups in a molecule and an organohydrogen polysiloxane having at least 3 silicon-bonded hydrogen atoms in a molecule in the presence of a condensation catalyst.

In the present invention, it is preferable that the silicone elastomer is used as a disperse solution thereof.
Method to prepare the silicone elastomer disperse solution is not particularly restricted; a heretofore known method to prepare a silicone elastomer disperse solution may be used. For example, the disperse solution may be produced by emulsifying a curable liquid silicone composition into water by using a surfactant, which is followed by a curing reaction of the resulting emulsion. For example, in the case of producing the silicone elastomer by curing with an addition reaction, the disperse solution may be produced by emulsifying a curable liquid silicone composition comprising the organopolysiloxane having olefinic unsaturated groups and the organohydrogen polysiloxane by adding a surfactant and water, which is followed by adding a platinum-based catalyst to conduct an addition polymerization of the resulting emulsion.

Alternatively, a curable liquid silicone composition obtained by an emulsion polymerization may be used. For example, in the case of forming the silicone elastomer by curing with a condensation reaction, into a cyclopolysiloxane shown by the general formula [R⁵ ₂SiO]_m (R⁵ represents a substituted or an unsubstituted monovalent hydrocarbon group having 1 to 30 carbon atoms, and "m" represents a number of 3 to 7) are added a surfactant and water for emulsification; and after a polymerization reaction of the obtained mixture is carried out by adding an acid, an alkali is added thereinto for neutralization to obtain an emulsion of a linear organopolysiloxane having silicon-bonded hydroxyl groups at its both terminals. Thereafter, an organotrialkoxy silane and a condensation catalyst are added to this emulsion to carry out a polycondensation reaction.

Surfactant used for emulsification of the curable liquid silicone composition is not particularly restricted. Illustrative examples thereof include a nonionic surfactant such as a polyoxyethylene alkyl ether, a polyoxyethylene polyoxypropylene alkyl ether, a polyoxyethylene alkyl phenyl ether, a polyethylene glycol fatty acid ester, a sorbitan fatty acid ester, a polyoxyethylene sorbitan fatty acid ester, a polyoxyethylene sorbit fatty acid ester, a glycerin fatty acid ester, a polyoxyethylene glycerin fatty acid ester, a polyglycerin fatty acid ester, a propylene glycol fatty acid ester, a polyoxyethylene propylene glycol fatty acid ester, a polyoxyethylene castor oil, a polyoxyethylene cured castor oil, a polyoxyethylene cured castor oil fatty acid ester, a polyoxyethylene phytostanol ether, a polyoxyethylene phytosterol ether, a polyoxyethylene cholestanol ether, a polyoxyethylene cholesteryl ether, a polyoxyethylene alkyl amine, an alkyl alkanol amide, a sucrose fatty acid ester, a methylglycoside fatty acid ester, an alkyl polyglycoside, a linear or a branched organopolysiloxane modified with polyoxyethylene, a linear or a branched organopolysiloxane modified with polyoxyethylene polyoxypropylene, an organopolysiloxane co-modified with polyoxyethylene and an alkyl, a linear or a branched organopolysiloxane co-modified with polyoxyethylene polyoxypropylene and an alkyl, a linear or a branched organopolysiloxane modified with polyglycerin, and a linear or a branched organopolysiloxane co-modified with polyglycerin and an alkyl; an anionic surfactant such as an alkyl sulfate ester salt, a polyoxyethylene alkyl ether sulfate ester salt, a polyoxyethylene alkyl phenyl ether sulfate ester salt, a sulfate ester salt of a fatty acid alkylolamide, an alkylbenzene sulfonate, a polyoxyethylene alkyl phenyl ether sulfonate, an alpha-olefin sulfonate, an alpha-sulfo fatty acid ester salt, an alkyl naphthalene sulfonate, an alkly diphenyl ether disulfonate, an alkane sulfonate salt, an N-acyltaurine salt, a dialkyl sulfosuccinate, a monoalkyl sulfosuccinate, a polyoxyethylene alkyl ether sulfosuccinate, a fatty acid salt, a polyoxyethylene alkyl ether carboxylic acid salt, a N-acyl aminoacid salt, a monoalkyl phosphate ester salt, a dialkyl phosphate ester salt, and a polyoxyethylene alkyl ether phosphate ester salt; a cationic surfactant such as an alkyl trimethyl ammonium salt, a dialkyl dimethyl ammonium salt, a polyoxyethylene alkyl dimethyl ammonium salt, a dipolyoxyethylene alkyl methyl ammonium salt, a tripolyoxyethylene alkyl ammonium salt, an alkyl benzyl dimethyl ammonium salt, an alkyl pyridinium salt, a monoalkyl amine salt, a dialkyl amine salt, a trialkyl amine salt, and a monoalkylamide amine salt; and an amphoteric surfactant such as an alkyl dimethyl amine oxide, an alkyl dimethyl carboxybetaine, an alkylamide propyl dimethyl carboxybetaine, an alkyl hydroxysulfobetaine, and an alkyl carboxymethyl hydroxyethyl imidazolinium betaine.

These surfactants may be used singly or as a mixture of two or more of them combined appropriately. Preferable selection is made from the nonionic surfactants. Use amount of the surfactant is preferably in the range of 0.1 to 50 parts by mass relative to 100 parts by mass of the curable liquid silicone composition.

For emulsification, a general emulsification dispersing equipment may be used; and illustrative examples thereof include a centrifugal throwing-out type agitator of high-speed rotation such as a homodisper; a shearing type agitator of high-speed rotation such as a homomixer; a high-pressure, injection-type emulsification disperser such as a homogenizer; a colloid mill; and an ultrasonic emulsifier.

It is preferable that the silicone elastomer disperse solution thus obtained is used as it stands without solid-liquid separation.

<Mixed aqueous disperse solution in which the inorganic powder and the silicone elastomer are dispersed >
The mixed aqueous disperse solution in which the inorganic powder and the silicone elastomer are dispersed may be obtained, for example, by mixing the inorganic powder, the silicone elastomer disperse solution, and as appropriate, water.

Adding amount of the inorganic powder is preferably in the range of 3 to 150 parts by mass, or more preferably 5 to 50 parts by mass, relative to 100 parts by mass of water blended therein. If the amount is 3 or more parts by mass, production efficiency thereof is good; on the other hand, if the amount is 150 or less parts by mass, dynamic viscosity of the aqueous mixed disperse solution is not too high so that adhesion of the silicone elastomer to the inorganic powder can be made readily. Alternatively, the inorganic powder prepared as a disperse solution in advance may be used as well.

Amount of the silicone elastomer is not particularly restricted in the case of expressing its adding effect to a cosmetic; however, if an excellent use feeling, such as a more remarkable soft focus effect, non-stickiness, smoothness, spreading properties, moistness, and softness, is desired, the amount thereof is preferably 0.5 or more parts by mass, more preferably 1 or more parts by mass, or still more preferably 2 or more parts by mass, relative to 100 parts by mass of the inorganic powder. If amount of the silicone elastomer is too large, higher degree of agglomeration may result whereby causing deterioration in spreading properties and in a use feeling such as non-stickiness and smoothness in a certain case; and thus, the amount thereof is preferably 100 or less parts by mass, more preferably 70 or less parts by mass, or still more preferably 50 or less parts by mass, relative to 100 parts by mass of the inorganic powder.

<Cationic water-soluble polymer>
In the present invention, a cationic water-soluble polymer is added into the aqueous mixed disperse solution in which the inorganic powder and the silicone elastomer are dispersed. If a cationic water-soluble polymer is used, the polymer assists adsorption of the silicone elastomer onto the inorganic powder so that the silicone elastomer can be uniformly adhered onto surface of the inorganic powder without agglomeration of the silicone elastomer.

Here, the cationic water-soluble polymer is a water-soluble polymer having a cationic group in its molecular structure; specifically, the cationic group thereof is a quaternary ammonium salt or an amino group. The cationic water-soluble polymer used in the present invention is not particularly restricted; but a synthetic type thereof whose polymer skeleton is synthesized by a vinyl polymerization, an addition polymerization, a condensation, and so on is preferable. In addition, it is preferable that neither an anionic group nor an amphoteric group is contained therein. If the cationic water-soluble polymer like this is used, the polymer assists adsorption of the silicone elastomer onto the inorganic powder so that the silicone elastomer can be uniformly adhered onto surface of the inorganic powder without agglomeration of the silicone elastomer; and thus, a cosmetic having a good use feeling such as smoothness and non-stickiness can be provided. The average molecular weight thereof is 5,000 to 10,000,000, or preferably 10,000 to 1,000,000.

Illustrative examples of the cationic water-soluble polymer include a polymer of dimethyl diallyl ammonium chloride; a copolymer of dimethyl diallyl ammonium chloride and acrylamide; a copolymer of dimethyl diallyl ammonium chloride, vinyl imidazoline, and vinyl pyrrolidone; a polymer of vinyl imidazoline; a polymer of methyl vinyl imidazolium chloride; a copolymer of methyl vinyl imidazolium chloride and vinyl pyrrolidone; a copolymer of methyl vinyl imidazolium methylsulfate, vinyl pyrrolidone, and vinyl caprolactam; a copolymer of methyl vinyl imidazolium chloride, vinyl imidazoline, vinyl pyrrolidone, and mathacrylic acid amide; a polymer of acrylic acid ethyl trimethyl ammonium chloride; a copolymer of acrylic acid ethyl trimethyl ammonium chloride and vinyl pyrrolidone; a copolymer of acrylic acid ethyl trimethyl ammonium chloride and acryl amide; a polymer of methacrylic acid ethyl trimethyl ammonium chloride; a copolymer of methacrylic acid ethyl trimethyl ammonium methylsulfate and acryl amide; a copolymer of methacrylic acid ethyl trimethyl ammonium chloride and methyl methacrylate; a copolymer of methacrylic acid ethyl trimethyl ammonium sulfate, dimethyl acrylamide, and dimethacrylic acid polyethylene glycol; a copolymer of methacrylic acid ethyl trimethyl ammonium chloride, acrylamide propyl trimethyl ammonium chloride, and dimethyl acrylamide; a copolymer of methacrylic acid ethyl trimethyl ammonium chloride, acrylamide propyl trimethyl ammonium chloride, dimethyl acrylamide, and methacrylic acid hydroxyethyl; a polymer of acrylamide propyl trimethyl ammonium chloride; a copolymer of acrylamide propyl trimethyl ammonium chloride and acrylamide; a copolymer of acrylamide propyl trimethyl ammonium chloride, dimethyl acrylamide, and methacrylic acid hydroxyethyl; a polymer of methacrylamide propyl trimethyl ammonium chloride; a copolymer of methacrylamide propyl trimethyl ammonium chloride and vinyl pyrrolidone; a polymer of ethylene imine; a quaternary compound of polyethylene imine; a polymer of allylamine hydrochloride salt; and polylysine. These may be used singly or as a mixture of two or more of them combined appropriately.

In order to make the silicone elastomer adhered more uniformly onto surface of the inorganic powder and to further enhance the providing effect of various properties to a cosmetic, it is preferable not to use a monomer which has a nonionic group; illustrative examples of the preferable polymer thereof include a polymer of dimethyl diallyl ammonium chloride, a polymer of vinyl imidazoline, a polymer of methyl vinyl imidazolium chloride, a polymer of acrylic acid ethyl trimethyl ammonium chloride, a polymer of methacrylic acid ethyl trimethyl ammonium chloride, a polymer of acrylamide propyl trimethyl ammonium chloride, a polymer of methacrylamide propyl trimethyl ammonium chloride, a polymer of ethylene imine, a quaternary compound of a polymer of ethylene imine, a polymer of allylamine hydrochloride salt, and polylysine.

Particularly preferable is a polymer of dimethyl diallyl ammonium chloride.
The polymer of dimethyl diallyl ammonium chloride can make the silicone elastomer adhered on surface of the inorganic powder more uniformly.

The cationic water-soluble polymer may be blended as it stands or as an aqueous solution into the mixed aqueous disperse solution in which the inorganic powder and the silicone elastomer are dispersed. The order of blending is not particularly restricted; the cationic water-soluble polymer may be blended and dissolved into water in advance, and then the mixed aqueous disperse solution in which the inorganic powder and the silicone elastomer are dispersed may be added thereinto.

Adding amount of the cationic water-soluble polymer is preferably in the range of 0.0001 to 1 part by mass relative to 100 parts by mass of water in the mixed aqueous disperse solution. If the adding amount is in the range of 0.0001 to 1 part by mass, more unifromly adhered silicone elastomer to surface of the inorganic powder may be obtained and state of the adhesion thereof may be made better. More preferable range thereof is in the range of 0.001 to 0.1 part by mass.

<Alkaline substance>
In the method for producing a composite particle of the present invention, an alkaline substance is used in addition.
The alkaline substance is used as a catalyst for the hydrolysis-condensation reaction of an alkoxy silane, a silanol group-containing silane, and a partial condensate of them.

It is preferable that the alkaline substance is added into water in which the inorganic powder and the silicone elastomer are dispersed and the cationic water-soluble polymer is dissolved. The order of blending them is not particularly restricted; the alkaline substance may be dissolved into water in advance, and then other components may be blended thereinto, or as a matter of course, the alkaline substance may be added after a part of other components are charged, and then rest of the components may be successively added thereinto.

Adding amount of the alkaline substance is such that pH of a mixed solution, comprising at least the alkaline substance and the mixed aqueous disperse solution in which the inorganic powder and the silicone elastomer are dispersed, may become preferably in the range of 10.0 to 13.0, or more preferably 10.5 to 12.5. If the alkaline substance is blended with the amount such that the said pH may become in the range of 10.0 to 13.0, the hydrolysis-condensation reaction of a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them as described later may take place sufficiently well.

The alkaline substance is not particularly restricted. Illustrative examples thereof include an alkaline metal hydroxide such as potassium hydroxide, sodium hydroxide, and lithium hydroxide; an alkaline earth metal hydroxide such as calcium hydroxide and barium hydroxide; an alkaline metal carbonate such as potassium carbonate and sodium carbonate; ammonia; a tetraalkyl ammonium hydroxide such as tetramethyl ammonium hydroxide and tetraethyl ammonium hydroxide; and an amine such as monomethyl amine, monoethyl amine, monopropyl amine, monobutyl amine, monopentyl amine, dimethyl amine, diethyl amine, trimethyl amine, triethanol amine, and ethylene diamine.

Among them, ammonia is most preferable because it can be easily removed from obtained silicone microparticle powders by evaporation. Ammonia of a commercially available aqueous ammonium solution may be used.

<Alkoxy silane, silanol group-containing silane, and partial condensate of them>
In the present invention, into the mixed solution of the cationic water-soluble polymer, the alkaline substance, and the mixed aqueous disperse solution in which the inorganic power and the silicone elastomer are dispersed are added further a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them.
The alkoxy silane, the silanol group-containing silane, and the partial condensate of them undergo a hydrolysis-condensation reaction by the catalytic action of the foregoing alkaline substance to give a resinous silicone (silicone resin).

In the present invention, the silicone resin like this is used as a binder between the inorganic powder and the silicone elastomer. In a composite particle having the silicone elastomer adhered onto surface of the inorganic powder by using the silicone resin as a binder, the silicone elastomer is firmly adhered onto surface of the inorganic powder so that it may not be removed from the powder surface readily whereby enhancing uniformity of the silicone elastomer adhesion; and as a result, much better use feeling can be provided. The silicone resin may be adhered onto a partial or an entire surface of any one of the inorganic powder and the silicone elastomer or both.

The silicone resin of the present invention is a polymer which comprises one, or two or more structure units selected from [R⁶SiO_3/2], [R⁶ ₂SiO_2/2], [R⁶ ₃SiO_1/2], and [SiO_4/2], while containing at least [R⁶SiO_3/2] or [SiO_4/2]. Here, each R⁶ independently represents a monovalent organic group having 1 to 20 carbon atoms. The silicone resin is produced, as mentioned later, by the hydrolysis-condensation reaction of a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them with having a silanol group remained because a part of them does not undergo the condensation reaction; and thus, accurately, the resin is a copolymer which contains a structure unit selected from the following structure units containing the silanol group.

Chemical formula 1

The alkoxy silane used in the present invention is shown by the general formulae R⁶Si(OR⁷)₃, R⁶ ₂Si(OR⁷)₂, R⁶ ₃SiOR⁷, and Si(OR⁷)₄. In these formulae, each R⁶ represents the same as before. Illustrative examples of R⁶ include an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, a nonyl group, a decyl group, a undecyl group, a dodecyl group, a tridecyl group, a tetradecyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, and an eicosyl group; a cycloalkyl group such as a cyclobutyl group, a cyclopentyl group, a cyclohexyl group, and a cycloheptyl group; an aryl group such as a phenyl group, a tolyl group, and a naphthyl group; an aralkyl group such as a benzyl group, a phenethyl group, and a beta-phenylpropyl group; an alkenyl group such as a vinyl group and an allyl group; and a hydrocarbon group whose part or all of hydrogen atoms bonded to a carbon atom of these groups is substituted with an atom such as a halogen atom (fluorine atom, chlorine atom, bromine atom, and iodine atom) and/or a substituent group, while illustrative examples of the said substituent group include an acryloyloxy group, a methacryloyloxy group, an epoxy group, a glycidoxy group, an amino group, a mercapto group, and a carboxyl group. The resinous silicone is produced by the hydrolysis-condensation reaction of a compound selected from the alkoxy silane, the silanol group-containing silane, and the partial condensate of them as described later, while in view of reactivity in the condensation, a methyl group is contained in R⁶ with the amount thereof being preferably 50% or more by mole, or more preferably 70% or more by mole. R⁷ represents an unsubstituted monovalent hydrocarbon group having 1 to 6 carbon atoms; and illustrative examples of R⁷ include a methyl group, an ethyl group, a propyl group, a butyl group, a pentyl group, and a hexyl group, though a methyl group is preferable in view of its reactivity.

Each of the alkoxy silanes shown by R⁶Si(OR⁷)₃, R⁶ ₂Si(OR⁷)₂, R⁶ ₃SiOR⁷, and Si(OR⁷)₄ becomes a source of the respective structure units shown by [R⁶SiO_3/2], [R⁶ ₂SiO_2/2], [R⁶ ₃SiO_1/2], and [SiO_4/2] in the resinous silicone.

If a resinous, solid material is desired, the structural body needs to contain the units [R⁶SiO_3/2] or [SiO_4/2]. The ratio, degree of polymerization, and hardness of the foregoing structural units are not particularly restricted, provided that the structural body contains at least the units [R⁶SiO_3/2] or [SiO_4/2] and that the resin is resinous solid at room temperature and not soluble in an oil substance used in a cosmetic as described later. However, if its melting point is too low, composite particles are melt-adhered with each other during a drying process or storage under atmosphere of a high temperature; and thus, the melting point thereof is preferably 50 degrees C or higher, or more preferably 80 degrees C or higher.

If amount of the [SiO_4/2] unit is too large, a sliding property decreases; and thus, a polymer comprising one, or two or more kinds, selected from [R⁶SiO_3/2], [R⁶ ₂SiO_2/2], and [R⁶ ₃SiO_1/2], and always containing [R⁶SiO_3/2], is preferable; the polymer containing 50% or more by mole of [R⁶SiO_3/2] is preferable, or more preferably 70% or more by mole.

Accordingly, the blending ratio of R⁶Si(OR⁷)₃, R⁶ ₂Si(OR⁷)₂, R⁶ ₃SiOR⁷, and Si(OR⁷)₄ may be determined such that a desired structure of the resinous silicone may be obtained. That is, the mole ratio is determined by the following relationship in considering a desired structural unit:
[R⁶SiO_3/2]:[R⁶ ₂SiO_2/2]:[R⁶ ₃SiO_1/2]:[SiO_4/2]= R⁶Si(OR⁷)₃:R⁶ ₂Si(OR⁷)₂:R⁶ ₃SiOR⁷:Si(OR⁷)₄

The silanol group-containing silane is the foregoing alkoxy silanes whose R⁷ in their general formulae is a hydrogen atom. The alkoxy silane, the silanol group-containing silane, and a condensate of them may be selected appropriately so as to obtain desired structural units.

A compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into an aqueous mixture containing an inorganic powder, a silicone elastomer, a cationic water-soluble polymer, and an alkaline substance with stirring the mixture to carry out the hydrolysis-condensation reaction. The compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them may be added gradually, or as a form dissolved in water or as a form dispersed in water, or as a blend with a water-soluble organic solvent such as an alcohol.

It is desirable that agitation thereof is made gently by using a puddle blade, a propeller blade, a sweptback blade, an anchor blade, and so on because vigorous agitation causes agglomeration of inorganic particles with each other, though agitation strength to satisfactorily disperse the inorganic powder and the compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them into the mixture solution is necessary.

Temperature during the time of adding the compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them into the mixture solution is preferably in the range of 0 to 60 degrees C, or more preferably 0 to 39 degrees C. If the temperature is 0 degrees C or higher, solidification of the mixture solution can be avoided; if the temperature is 60 degrees C or lower, agglomeration of the particles obtained does not take place.

By the hydrolysis-condensation reaction, the resinous silicone is formed on the inorganic powder surface and/or the silicone elastomer surface whereby the inorganic powder is adhered with the silicone elastomer to form a composite particle having the inorganic powder surface adhered with the silicone elastomer by using the silicone resin as a binder.

Amount of the compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is not particularly restricted; but in order to uniformly adhere the silicone elastomer onto surface of the inorganic powder and to enhance adhesion strength of the silicone elastomer to the inorganic powder, the amount thereof is preferably 10 or more parts by mass, more preferably 20 or more parts by mass, or still more preferably 30 or more parts by mass, relative to 100 parts by mass of the silicone elastomer. If amount of the silicone resin is too large, there is a certain case that a soft feeling of the silicone elastomer may not be expressed; and thus, the amount thereof is preferably 500 or less parts by mass, more preferably 300 or less parts by mass, or still more preferably 200 or less parts by mass, relative to 100 parts by mass of the silicone elastomer.

With an aim to uniformly adhere the silicone elastomer onto surface of the inorganic powder, a water-soluble organic solvent such as an alcohol may be added into the mixed solution. In the case of obtaining a particle whose surface is treated with a silylation agent, a composite particle already produced may be treated; or alternatively, a silylation agent may be added to conduct the surface treatment after the compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into the mixed solution. Illustrative examples of the silylation agent include dimethyl dichloro silane, trimethyl chloro silane, trimethyl methoxy silane, silane containing trimethyl silanol group, and hexamethyl disilazane.

After completion of addition of the compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them, it is preferable that the resulting mixture is agitated for a while until completion of the hydrolysis-condensation reaction. In order to accelerate the reaction, the mixture may be heated at 40 to 100 degrees C, or an alkaline substance may be added additionally. Thereafter, an acidic substance may be added for neutralization, if necessary.

After the hydrolysis-condensation reaction, water is removed. Water may be removed, for example, by heating the mixture solution after the reaction under normal pressure or reduced pressure; specific examples of the method include a method to remove water by heating the mixture solution under a static condition, a method to remove water by heating the mixture solution under fluidized condition by agitation, a method to spray and disperse the mixture solution into a hot air stream such as a spray dryer, and a method using a fluid heating medium. Meanwhile, as the pre-treatment of this operation, the mixture solution may be concentrated by thermal dehydration, filtration by a filter press and the like, centrifugal separation, decantation, and so on; the mixture solution may also be rinsed with water, an alcohol, or the like, if necessary.

If the powders obtained by removing water from the mixture solution after the reaction are agglomerated, the powders may be crushed by a crushing equipment such as a jet mill, a ball mill, and a hammer mill, or classified.

The composite particle obtained by the present invention is a particle having the silicone elastomer adhered on surface of the inorganic powder by using the silicone resin as a binder; but in order to provide or improve water-repellent properties and to improve dispersibility into an oil material, surface of the particle may be treated with a silylation agent, a silicone oil, a wax, a paraffin, an organic fluorinated compound, a surfactant, and so on.
State of the inorganic powder whose surface is adhered with the silicone elastomer may be confirmed by an electron microscope.

II. A method for producing a cosmetic by using the composite particle
In the method for producing a cosmetic of the present invention, a cosmetic is produced by using the composite particle (hereinafter, designated by (A)) which is produced by the method for producing the composite particle of the present invention and has the silicone elastomer adhered onto surface of the inorganic powder by using the silicone resin as a binder.
More specifically, an intended cosmetic is produced by using the composite particle (A) and later-mentioned various cosmetic ingredients, all of which are then subjected to mixing, emulsifying, and so on.

III. A cosmetic containing the composite particle
A cosmetic of the present invention is characterized in that the cosmetic contains the composite particle (namely the composite particle (A)) produced by a hydrolysis-condensation reaction of a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them added into a mixed solution containing a cationic water-soluble polymer, an alkaline substance, and an aqueous mixture disperse solution in which an inorganic powder and a silicone elastomer are dispersed, thereby forming the composite particle having the silicone elastomer adhered onto surface of the inorganic powder by using a silicone resin as a binder. Blending ratio of the composite particle (A) is not particularly limited; it is selected appropriately, in accordance with respective ingredients, from the range of 0.1 to 95.0% by mass relative to totality of the cosmetic.

The cosmetic of the present invention may be blended with various ingredients used in an ordinary cosmetic, in addition to the composite particle (A). Illustrative examples of the ingredients include (B) an oil material, (C) water, (D) a compound having an alcoholic hydroxyl group, (E) a water-soluble or a water-swelling polymer, (F) a particle other than the composite particle (A) in the cosmetic of the present invention, (G) a surfactant, (H) a composition comprising a crosslinking organopolysiloxane and an oil material which is in the state of liquid at room temperature, (I) a silicone resin, (J) a silicone wax, and other additives. These may be used singly or as an appropriate combination of two or more of them.

The oil material (B) may be in the form of any of a solid, a semi-solid, and a liquid. For example, a natural animal or a vegetable oil fat, a semi-synthetic oil fat, a hydrocarbon oil, a higher alcohol, an ester oil, a silicone oil, and a fluorinated oil material may be used.
Illustrative examples of the natural animal and vegetable oil fat and the semi-synthetic oil fat include an avocado oil, a linseed oil, an almond oil, an insects wax, a perilla oil, an olive oil, a cocoa butter, a kapok wax, a kaya oil, a carnauba wax, a lever oil, a candellila wax, a purified candellila wax, a beef tallow, a neats-foot oil, a beef bone fat, a cured beef tallow, an apricot kernel oil, a whale wax, a hydrogenated oil, a wheat germ oil, a sesame oil, a rice germ oil, a rice bran oil, a sugarcane wax, a sasanqua oil, a safflower oil, a shea butter, a Chinese tung oil, a cinnamon oil, a jojoba wax, squalane, squalene, a shellac wax, a turtle oil, a soybean oil, a tea seed oil, a camellia oil, an evening primrose oil, a corn oil, a pig fat, a rapeseed oil, a Japanese tung oil, a bran wax, a germ oil, a horse fat, a persic oil, a palm oil, a palm kernel oil, a castor oil, a cured castor oil, a methyl ester of cured castor oil fatty acid, a sunflower oil, a grape seed oil, a bayberry wax, a jojoba oil, a macadamia nut oil, a bees wax, a mink oil, a meadowfoam seed oil, a cotton seed oil, a cotton wax, a Japan wax, a Japan wax kernel oil, a montan wax, a coconut oil, a cured coconut oil, a tri-coconut fatty acid glyceride, a mutton tallow, a peanut oil, lanolin, liquid lanolin, reduced lanolin, lanolin alcohol, hard lanolin, lanolin acetate, lanolin alcohol acetate, isopropyl lanolin fatty acid, polyoxyethylene lanolin alcohol ether, polyoxyethylene lanolin alcohol acetate, polyethylene glycol lanolin fatty acid, polyoxyethylene hydrogenated lanolin alcohol ether, and an egg-yolk oil.

Illustrative examples of the hydrocarbon oil include a linear and a branched hydrocarbon oil; and it may be a volatile hydrocarbon oil and a non-volatile hydrocarbon oil. Specific examples thereof include an ozocerite, an alpha-olefin oligomer, a light isoparaffin, isododecane, isohexadecane, a light liquid isoparaffin, squalane, a synthetic squalane, a vegetable squalane, squalene, a ceresin, a paraffin, a paraffin wax, a polyethylene wax, a polyethylene/polypropylene wax, ethylene/propylene/styrene copolymer, butylene/propylene/styrene copolymer, a liquid paraffin, a liquid isoparaffin, a pristane, polyisobutylene, a hydrogenated isobutene, a microcrystalline wax, and vaseline. Illustrative examples of the higher fatty acid include lauric acid, myristic acid, palmitic acid, stearic acid, behenic acid, undecylenic acid, oleic acid, linoleic acid, linolenic acid, arachidonic acid, eicosapentaenoic acid (EPA), docosahexaenoic acid (DHA), isostearic acid, and 12-hydroxystearic acid.

Illustrative examples of the higher alcohol include an alcohol having preferably 6 or more carbon atoms, or more preferably 10 to 30 carbon atoms. Specific examples of the higher alcohol include lauryl alcohol, myristyl alcohol, palmityl alcohol, stearyl alcohol, behenyl alcohol, hexadecyl alcohol, oleyl alcohol, isostearyl alcohol, hexyl dodecanol, octyl dodecanol, cetostearyl alcohol, 2-decyl tetradecynol, cholesterol, phytosterol, polyoxyethylene cholesterol ether, monostearyl glycerin ether (batyl alcohol), and monooleyl glyceryl ether (selachyl alcohol).

Illustrative examples of the ester oil include diisobutyl adipate, 2-hexyldecyl adipate, di-2-heptylundecyl adipate, an N-alkylglycol monoisostearate, isocetyl isostearate, trimethylolpropane triisostearate, ethylene glycol di-2-ethylhexanoate, cetyl 2-ethylhexanoate, trimethylolpropane tri-2-ethylhexanoate, pentaerythritol tetra-2-ethylhexanoate, cetyl octanoate, octyl dodecyl gum ester, oleyl oleate, octyldodecyl oleate, decyl oleate, neopentyl glycol dioctanoate, neopentyl glycol dicaprate, triethyl citrate, 2-ethylhexyl succinate, amyl acetate, ethyl acetate, butyl acetate, isocetyl stearate, butyl stearate, diisopropyl sebacate, di-2-ethylhexyl sebacate, cetyl lactate, myristyl lactate, isononyl isononanoate, isotridecyl isononanoate, isopropyl palmitate, 2-ethylhexyl palmitate, 2-hexyldecyl palmitate, 2-heptylundecyl palmitate, cholesteryl 12-hydroxystearate, a dipentaerythritol fatty acid ester, isopropyl myristate, octyldodecyl myristate, 2-hexyldecyl myristate, myristyl myristate, hexyldecyl dimethyloctanoate, ethyl laurate, hexyl laurate, 2-octyldodecyl N-lauroyl-L-glutamate ester, isopropyl lauroylsarcosinate ester, and diisostearyl malate; and a glyceride oil such as acetoglyceryl, glyceryl triisooctanoate, glyceryl triisostearate, glyceryl triisopalmitate, glyceryl tribehenate, glyceryl monostearate, glyceryl di-2-heptylundecanoate, glyceryl trimyristate, and diglyceryl myristate isostearate.

Illustrative examples of the silicone oil include a linear or a branched organopolysiloxane having low to high viscosity such as dimethyl polysiloxane, tristrimethylsiloxy methyl silane, caprylyl methicone, phenyl trimethicone, tetrakistrimethylsiloxy silane, methyl phenyl polysiloxane, methyl hexyl polysiloxane, methyl hydrogen polysiloxane, and dimethylsiloxane/methyl phenyl siloxane copolymer; a cyclic organopolysiloxane such as octamethyl cyclotetrasiloxane, decamethyl cyclopentasiloxane, dodecamethyl cyclohexasiloxane, tetramethyl tetrahydrogen cyclotetrasiloxane, and tetramethyl tetraphenyl cyclotetrasiloxane; a silicone rubber such as an amino-modified organopolysiloxane, a pyrrolidone-modified organopolysiloxane, a pyrrolidone carboxylate-modified organopolysiloxane, a dimethyl polysiloxane gum of a high degree of polymerization, an amino-modified organopolysiloxane gum, and a dimethylsiloxane/methyl phenyl siloxane copolymer gum; a cyclic organopolysiloxane solution of a silicone gum or a silicone rubber, trimethylsiloxy silicic acid, a cyclic siloxane solution of trimethylsiloxy silicic acid, a higher alkoxy-modified silicone such as stearoxysilicone, a higher fatty acid-modified silicone, an alkyl-modified silicone, a long chain alkyl-modified silicone, an amino-modified silicone, a fluorine-modified silicone, a silicone resin, and a solution containing a dissolved silicone resin.

Illustrative examples of the fluorinated oil material include perfluoro polyether, perfluoro decalin, and perfluoro octane.
Amount of the oil material (B) to be blended is dependent on the form of the cosmetic; but it is appropriately selected from the range of 1 to 98% by mass relative to the totality of the cosmetic.

Amount of water (C) to be blended is dependent on the form of the cosmetic; but it is appropriately selected from the range of 1 to 95% by mass relative to the totality of the cosmetic.

Illustrative examples of the compound containing an alcoholic hydroxyl group (D) include a lower alcohol containing preferably 2 to 5 carbon atoms, such as ethanol and isopropanol; and a sugar alcohol such as sorbitol and maltose. In addition, illustrative examples thereof include a sterol such as cholesterol, sitosterol, phytosterol, and lanosterol; and a polyvalent alcohol such as butylene glycol, propylene glycol, dibutylene glycol, and pentylene glycol. Amount thereof to be blended is selected appropriately from the range of 0.1 to 98% by mass relative to the totality of the cosmetic.

Illustrative examples of the water-soluble or water-swelling polymer (E) include a plant polymer such as an Arabia gum, tragacanth, galactan, a carob gum, a guar gum, a karaya gum, carrageenan, pectin, agar, quince seed (marmelo), starch (rice, corn, potato, wheat, and so on), an algae colloid, a trant gum, and a locust bean gum; a microbial polymer such as a xanthan gum, dextran, succinoglucan, and pullulan; an animal polymer such as collagen, casein, albumin, and gelatin; a starch polymer such as carboxymethyl starch and methylhydroxypropyl starch; a cellulose polymer such as methyl cellulose, ethyl cellulose, methyl hydroxypropyl cellulose, carboxymethyl cellulose, hydroxymethyl cellulose, hydroxypropyl cellulose, nitrocellulose, sodium cellulose sulfate, sodium carboxymethyl cellulose, crystalline cellulose, and cellulose powder; an alginic acid polymer such as sodium alginate and propylene glycol alginate ester; a vinyl polymer such as polyvinyl methyl ether and carboxy vinyl polymer; a polyoxyethylene polymer; a polyoxyethylene polyoxypropylene copolymer; an acryl polymer such as sodium polyacrylate, polyethyl acrylate, polyacrylamide, and an acryloyldimethyl taurate salt copolymer; other synthetic water-soluble polymer such as polyethyleneimine and an cationic polymer; and an inorganic water-soluble polymer such as bentonite, aluminum magnesium silicate, montomorillonite, beidellite, nontronite, saponite, hectorite, and anhydrous silicic acid. In addition, a film-forming material such as polyvinyl alcohol and polyvinyl pyrrolidone is included in the water-soluble polymer. Amount of these polymers to be blended is preferably in the range of 0.1 to 25% by mass relative to the totality of the cosmetic.

Illustrative examples of the particle (F) other than the composite particle (A) in the cosmetic of the present invention include an inorganic particle, an organic particle, an inorganic-organic composite powder, and a silicone resin particle.
Illustrative examples of the inorganic particle include the same as those mentioned in the method for producing the composite particle of the present invention.

Illustrative examples of the organic particle include a powder of polyamide, polyacrylic acid-polyacrylate ester, polyester, polyethylene, polypropylene, polystyrene, styrene-acrylic acid copolymer, divinyl benzene-styrene copolymer, polyurethane, vinyl resin, urea resin, melamine resin, bezoguanamine, polymethyl benzoguanamine, tetrafluoroethylene, polymethyl methacrylate (such as for example, methyl polymethacrylate), cellulose, silk, nylon, phenolic resin, epoxy resin, and polycarbonate resin.

In addition, illustrative examples of the organic particle include a surfactant metal salt powder (metal soap); and specific examples thereof include a powder of zinc stearate, aluminum stearate, calcium stearate, magnesium stearate, zinc myristate, magnesium myristate, zinc cetylphosphate, calcium cetylphosphate, and sodium cetylphosphate zinc.

Further in addition, illustrative examples of the organic particle include an organic dye; and specific examples thereof include a tar dye such as Red No. 3, Red No. 104, Red No. 106, Red No. 201, Red No. 202, Red No. 204, Red No. 205, Red No. 220, Red No. 226, Red No. 227, Red No. 228, Red No. 230, Red No. 401, Red No. 505, Yellow No. 4, Yellow No. 5, Yellow No. 202, Yellow No. 203, Yellow No. 204, Yellow No. 401, Blue No. 1, Blue No. 2, Blue No. 201, Blue No. 404, Green No. 3, Green No. 201, Green No. 204, Green No. 205, Orange No. 201, Orange No. 203, Orange No. 204, Orange No. 206, and Orange No. 207; and a natural dye such as carminic acid, laccaic acid, carthamin, brazilin, and crocin.

Illustrative examples of the inorganic-organic composite powder include a composite powder having surface of an inorganic powder widely used in a cosmetic covered with an organic powder by a heretofore known method.

Illustrative examples of the silicone resin particle include a silicone elastomer particle, a polymethyl silsesquioxane particle (specific examples thereof include KMP-590 and 591, manufactured by Shin-Etsu Chemical Co., Ltd.), and a particle having surface of a silicone elastomer particle covered with polymethyl silsesquioxane (specific examples thereof include KSP-100, 101, 102, 105, 300, 411, and 441).

As to the particle other than the composite particle (A) in the cosmetic of the present invention, particle whose surface is treated with a silane or a silylation agent such as capryl silane (AES-3083, manufactured by Shin-Etsu Chemical Co., Ltd.), with a silicone oil such as dimethyl silicone (KF-96AK series, manufactured by Shin-Etsu Chemical Co., Ltd.), polysiloxane of a methylhydrogen type (KF-99P, KF-9901, and so on, manufactured by Shin-Etsu Chemical Co., Ltd.), and a silicone-treating agent of a silicone branching type (KF-9908, KF-9909, and so on, manufactured by Shin-Etsu Chemical Co., Ltd.), with a wax, with a paraffin, with an organic fluorinated compound such as a phosphate of a perfluoroalkyl, with a surfactant, with an amino acid such as N-acylglutamic acid, and with a metal soap such as aluminum stearate and magnesium myristate may be used. Blending amount thereof is not particularly restricted; and thus, there may be the case that the amount is nearly 100% relative to totality of the cosmetic.

As to the surfactant (G), there are a nonionic, an anionic, a cationic, and an amphoteric surfactant; illustrative examples thereof include the same surfactants as those used in the method for preparation of the silicone elastomer disperse solution as mentioned before. Among those surfactants, preferable are a linear or a branched organopolysiloxane modified with polyoxyethylene, a linear or a branched organopolysiloxane modified with polyoxyethylene polyoxypropylene, a linear or a branched organopolysiloxane co-modified with polyoxyethylene and an alkyl, a linear or a branched organopolysiloxane co-modified with polyoxyethylene polyoxypropylene and an alkyl, a linear or a branched organopolysiloxane modified with polyglycerin, and a linear or a branched organopolysiloxane co-modified with polyglycerin and an alkyl. In these surfactants, content of the hydrophilic group of a polyoxyethylene group, a polyoxyethylene polyoxypropylene group, or a polyglycerin residue is preferably in the range of 10 to 70% by mass in its molecular structure. Specific examples of them include KF-6011, 6043, 6028, 6038, 6100, 6104, and 6105 (manufactured by Shin-Etsu Chemical Co., Ltd.). Blending amount thereof is preferably in the range of 0.1 to 20% by mass, or more preferably 0.2 to 10% by mass, relative to totality of the cosmetic. HLB of the surfactant is not particularly restricted, but preferably in the range of 2 to 14.5.

In the composition comprising a crosslinking organopolysiloxane and an oil material which is in the state of liquid at room temperature (H), it is preferable that this crosslinking organopolysiloxane swells by absorbing the liquid oil with the amount thereof being more than own weight of the crosslinking organopolysiloxane. Here, as the liquid oil, a liquid oil in the oil material (B), namely, a silicone oil, a hydrocarbon oil, an ester oil, a natural vegetable and an animal oil, a semi-synthetic oil, and a fluorinated oil may be used; and illustrative examples thereof include a low viscous silicone oil having viscosity of 0.65 to 100 mm²/second (at 25 degrees C); a hydrocarbon oil such as a liquid paraffin, squalane, isododecane, and isohexadecane; a glyceride oil such as trioctanoin; an ester oil such as isotridecyl isononanoate, an N-acyl glutamate ester, and lauroyl sarocosinate ester; and a natural vegetable and an animal oil such as a macadamia nut oil. It is preferable that the crosslinking agent of this crosslinking organopolysiloxane has two or more reactive vinyl moieties in its molecular structure and form a crosslinking structure by reacting with a hydrogen atom directly bonded to a silicon atom. Illustrative examples of the crosslinking agent having two or more reactive vinyl moieties in its molecular structure include an organopolysiloxane containing two or more vinyl groups in its molecular structure, a polyoxyalkylene containing two or more allyl groups in its molecular structure, a polyglycerin containing two or more allyl groups in its molecular structure, and an alpha, omega-alkenyl diene. Further, a crosslinking organopolysiloxane containing at least one moiety selected from the group consisting of a polyoxyalkylene moiety, a polyglycerin moiety, a long-chain alkyl moiety, an alkenyl moiety, an aryl moiety, and a fluoroalkyl moiety may be used. Specific examples thereof include a KSG series (trade name), especially KSG-15, 16, 41, 42, 43, 44, 042Z, and 045Z; and KSG-210, 710, 310, 320, 330, 340, 320Z, 350Z, 810, 820, 830, 840, 820Z, and 850Z (manufactured by Shin-Etsu Chemical Co., Ltd.). Amount of the composition comprising the crosslinking organopolysiloxane and the oil material which is in a liquid state at room temperature is, if it is used, preferably 0.1 to 80% by mass, or more preferably 1 to 50% by mass, relative to totality of the cosmetic.

As to the silicone resin (I), an acryl silicone resin of an acryl-silicone graft or block copolymer is preferable. It is also possible to use an acryl silicone resin containing at least one moiety selected from a pyrrolidone moiety, a long-chain alkyl moiety, a polyoxyalkylene moiety, a fluoroalkyl moiety, and an anionic moiety such as a carboxylic acid. Specific examples thereof include a cyclic organopolysiloxane solution of an acryl-silicone graft copolymer, such as KP-545 (manufactured by Shin-Etsu Chemical Co., Ltd.). This silicone resin is preferably a net-work silicone compound such as a resin composed of a R⁸ ₃SiO_0.5 unit and a SiO₂ unit; a resin composed of a R⁸ ₃SiO_0.5 unit, a R⁸ ₂SiO unit, and a SiO₂ unit; a resin composed of a R⁸ ₃SiO_0.5 unit and a R⁸SiO_1.5 unit; a resin composed of a R⁸ ₃SiO_0.5 unit, a R⁸ ₂SiO unit, and a R⁸SiO_1.5 unit; and a resin composed of a R⁸ ₃SiO_0.5 unit, a R⁸ ₂SiO unit, a R⁸SiO_1.5 unit, and a SiO₂ unit. Here, R⁸ in these formulae represents a substituted or an unsubstituted monovalent hydrocarbon group having 1 to 30 carbon atoms. Specific examples thereof include a cyclic siloxane solution of trimethyl siloxysilicic acid, such as KF-7312J (manufactured by Shin-Etsu Chemical Co., Ltd.). It is also possible to use a net-work silicone compound containing in its molecular structure at least one moiety selected from a pyrrolidone moiety, a long-chain alkyl moiety, a polyoxyalkylene moiety, a polyglycerin moiety, a fluoroalkyl moiety, and an amino moiety. When a silicone resin such as the acryl silicone resin and the net-work silicone compound is used, amount thereof to be blended is preferably 0.1 to 20% by mass, or more preferably 1 to 10% by mass, relative to totality of the cosmetic.

As to the silicone wax (J), an acryl silicone resin of an acryl-silicone graft or block copolymer is preferable. It is also possible to use an acryl silicone resin containing at least one moiety selected from a pyrrolidone moiety, a long-chain alkyl moiety, a polyoxyalkylene moiety, a fluoroalkyl moiety, and an anionic moiety such as a carboxylic acid. Specific examples thereof include an acryl-silicone graft copolymer, such as KP-561P and 562P (manufactured by Shin-Etsu Chemical Co., Ltd.). This silicone wax is preferably a polysiloxane modified with a polylactone by bonding a polylactone which is a ring-opened polymer of a lactone compound having 5 or more ring members. In addition, this silicone wax is a silicone-modified olefin wax obtained by an addition reaction of an olefin wax containing an unsaturated group comprising an alpha-olefin and diene with an organohydrogen polysiloxane containing one or more SiH bond in its molecular structure. As to the alpha-olefin of the olefin wax, those having 2 to 12 carbon atoms such as ethylene, propylene, 1-butene, 1-hexene, and 4-methyl-1-pentene are preferable; and as to the diene, butadiene, isoprene, 1,4-hexadiene, vinyl norbornene, ethylidene norbornene, dicyclopentadiene, and so on are preferable. As to the organohydrogen polysiloxane containing the SiH bond, those having a linear structure, a siloxane branched structure, and so on may be used. Amount of the silicone wax if it is used is preferably 0.1 to 30% by mass, or more preferably 1 to 10% by mass, relative to totality of the cosmetic.

Illustrative examples of the other additives include an oil-soluble gelation agent, an antiperspirant, a UV-absorber, a UV absorbing-scattering agent, a moisturizer, an antibacterial preservative, a fragrance, a salt, an antioxidant, a pH controller, a chelating agent, an algefacient, an anti-inflammatory agent, a skin care ingredient (a skin-lightening agent, a cell activator, a rough-skin improver, a blood circulation promoter, a skin astringent agent, an antiseborrheic agent, and so on), a vitamin, an amino acid, a nucleic acid, a hormone, a clathrate compound, and a hair-immobilizing agent.

Illustrative examples of the oil-soluble gelation agent include a metal soap such as aluminum stearate, magnesium stearate, and zinc myristate; an amino acid derivative such as N-lauroyl-L-glutamic acid and alpha, gamma-di-n-butyl amine; a dextrin fatty acid ester such as dextrin palmitate ester, dextrin stearate ester, and dextrin 2-ethylhexanoate palmitate ester; a sucrose fatty acid ester such as sucrose palmitate ester and sucrose stearate ester; a fructo-oligosaccharide fatty acid ester such as fructo-oligosaccharide stearate ester and fructo-oligosaccharide 2-ethylhexanoate ester; a benzylidene derivative of sorbitol such as monobenzylidene sorbitol and dibenzylidene sorbitol; and an organic-modified clay mineral such as dimethyl benzyl dodecyl ammonium montomorillonite clay and dimethyl dioctadecyl ammonium montomorillonite clay.

Illustrative examples of the antiperspirant include aluminum chlorohydrate, aluminum chloride, aluminum sesquichlorohydrate, zirconyl hydroxy chloride, aluminum zirconium hydroxy chloride, and aluminum zirconium glycine complex.

Illustrative examples of the UV-absorber include a benzoic acid UV-absorber such as para-amino benzoic acid; an anthranilic acid UV-absorber such as methyl anthranilate; a salicylic acid UV-absorber such as methyl salicylate, octyl salicylate, and trimethylcyclohexyl salicylate; a cinnamic acid UV-absorber such as octyl para-methoxy cinnamate; a benzophenone UV-absorber such as 2,4-dihydroxybenzophenone; a urocanic acid UV-absorber such as ethyl urocanate; a dibenzoylmethane UV-absorber such as 4-t-butyl-4'-methoxy-dibenzoylmethane; phenyl benzimidazole sulfonic acid; and a triazine derivative. Illustrative examples of the UV absorbing-scattering agent include a particle which absorbs and scatters a UV-ray, such as a titanium oxide microparticle, titanium oxide containing an iron microparticle, a zinc oxide microparticle, a cerium oxide microparticle, and a composite material of them. A dispersed material obtained by dispersing these particles which absorb and scatter a UV-ray into an oil material prior to use may also be used.

Illustrative examples of the moisturizer include glycerin, sorbitol, propylene glycol, dipropylene glycol, 1,3-butylene glycol, pentylene glycol, glucose, xylitol, maltitol, polyethylene glycol, hyaluronic acid, chondroitin sulfate, pyrrolidone carboxylate salt, polyoxyethylene methyl glucoside, polyoxypropylene methyl glucoside, egg yolk lecithin, soybean lecithin, phosphatidyl choline, phosphatidyl ethanolamine, phosphatidyl serine, phosphatidyl glycerol, phosphatidyl inositol, and sphingo phospholipid.

Illustrative example of the antibacterial preservative include a para-oxybenzoate alkyl ester, benzoic acid, sodium benzoate, sorbic acid, potassium sorbate, and phenoxy ethanol. Illustrative examples of the antibacterial agent include benzoic acid, salicylic acid, carbolic acid, sorbic acid, a para-oxybenzoate alkyl ester, p-chloro-m-cresol, hexachlorophene, benzalkonium chloride, chlorhexidine chloride, trichlorocarbanilide, a photosensitive element, and phenoxy ethanol.

As to the fragrance, there are a natural fragrance and a synthetic fragrance. As to the natural fragrance, there are a plant fragrance extracted from a flower, a leaf, a stem, a fruit skin, and so on, and an animal fragrance such as musk and civet. Illustrative examples of the synthetic fragrance include a hydrocarbon such as a monoterpene; an alcohol such as an aliphatic alcohol and an aromatic alcohol; an aldehyde such as a terpene aldehyde and an aromatic aldehyde; a ketone such as an alicyclic ketone; an ester such as a terpene ester; a lactone; a phenol; an oxide; a nitrogen-containing compound; and an acetal.

As to the salt, an inorganic salt, an organic acid salt, an amine salt, and an amino acid salt may be mentioned. Illustrative examples of the inorganic salt include a sodium, a potassium, a magnesium, a calcium, an aluminum, a zirconium, and a zinc salt of an inorganic acid such as hydrochloric acid, sulfuric acid, carbolic acid, and nitric acid. Illustrative examples of the organic acid salt include a salt of an organic acid such as acetic acid, dehydroacetic acid, citric acid, malic acid, succinic acid, ascorbic acid, and stearic acid. Illustrative examples of the amine salt and the amino acid salt include a salt of an amine such as triethanol amine and an amino acid salt such as a glutamate salt. In addition, a salt of hyaluronic acid and chondroitin sulfate, an aluminum zirconium glycine complex, and a neutralized salt obtained by neutralization of an acid and an alkali used in a cosmetic prescription may be used.

Illustrative examples of the antioxidant include tocopherol, p-t-butylphenol, butyl hydroxy anisole, dibutyl hydroxy toluene, and phytin; illustrative examples of the pH-controller include lactic acid, citric acid, glycolic acid, succinic acid, tartaric acid, dl-malic acid, potassium carbonate, sodium bicarbonate, and ammonium bicarbonate; illustrative examples of the chelating agent include alanine, sodium edetate, sodium polyphosphate, sodium metaphosphate, and phosphoric acid; illustrative examples of the algefacient include L-menthol and camphor; and illustrative examples of the anti-inflammatory agent include allantoin, glycyrrhizic acid and its salt, glycyrrhetic acid, stearyl glycyrrhetinate, tranexamic acid, and azulene.

Illustrative examples of the skin care ingredient include a skin-lightening agent such as a placenta extract, arbutin, glutathione, and a saxifrage extract; a cell activator such as a royal jelly, a photosensitive element, a cholesterol derivative, and an extract from hemolysed blood of a young calf; a rough-skin improver; a blood circulation promoter such as nonylic acid warenylamide, benzyl nicotinate ester, beta-butoxyethyl nicotinate ester, capsaicin, zingerone, cantharides tincture, ichthammol, caffeine, tannic acid, alpha-borneol, nicotinic acid tocopherol, inositol hexanicotinate, cyclandelate, cinnarizine, tolazoline, acetyl choline, verapamil, cepharanthin, and gamma-orizanol; a skin astringent agent such as zinc oxide and tannic acid; and an antiseborrheic agent such as sulfur and thianthrol.

Illustrative examples of the vitamin include a vitamin A such as a vitamin A oil, retinol, retinol acetate, and retinol palmitate; a vitamin B including a vitamin B₂ such as riboflavin, riboflavin butyrate, and a flavin adenine nucleotide, a vitamin B₆ such as pyridoxine hydrochloride salt, pyridoxine dioctanoate, and pyridoxine tripalmitate, a vitamin B₁₂ and its derivative, and vitamin B₁₅ and its derivative; a vitamin C such as L-ascorbic acid, L-ascorbic acid dipalmitate ester, sodium L-ascorbic-2-sulfate, and dipotassium L-ascorbic acid phosphate diester; a vitamin D such as ergocalciferol and cholecalciferol; a vitamin E such as alpha-tocopherol, beta-tocopherol, gamma-tocopherol, dl-alpha-tocopherol acetate, dl-alpha-tocopherol nicotinate, and dl-alpha-tocopherol succinate; a nicotinic acid such as nicotinic acid, benzyl nicotinate, and a nicotinic acid amide; a vitamin H; a vitamin P; a pantothenic acid such as calcium pantothenate, D-pantothenyl alcohol, pantothenyl ethyl ether, and acetyl pantothenyl ethyl ether; and biotin.

Illustrative examples of the amino acid include glycine, valine, leucine, isoleucine, serine, threonine, phenylalanine, arginine, lysine, aspartic acid, glutamic acid, cystine, cysteine, methionine, and tryptophan.

Illustrative examples of the nucleic acid include deoxyribonucleic acid.
Illustrative examples of the hormone include estradiol and ethinyl estradiol.
Illustrative examples of the clathrate compound include cyclodextrin.

As to the hair-immobilizing agent, an amphoteric polymer, an anionic polymer, a cationic polymer, and a nonionic polymer may be mentioned. Illustrative examples thereof include a polyvinyl pyrrolidone polymer such as polyvinyl pyrrolidone and vinyl pyrrolidone/vinyl acetate copolymer; an acidic vinyl ether polymer such as a methyl vinyl ether/maleic anhydride alkyl half-ester copolymer; an acidic polyvinyl acetate polymer such as vinyl acetate/crotonic acid copolymer; an acidic acryl polymer such as a (meth)acrylic acid/alkyl (meth)acrylate copolymer and a (meth)acrylic acid/alkyl (meth)acrylate/alkyl acrylamide copolymer; and an amphoteric acryl polymer such as a N-methacryloylethyl-N,N-dimethyl ammonium/alpha-N-methylcarboxybetaine/alkyl (meth)acrylate copolymer and hydroxypropyl (meth)acrylate/butylaminoethyl methacrylate/acrylic acid octyl amide copolymer. In addition, a polymer derived from a nature such as cellulose or its derivative, and keratin and collagen or a derivative of them may be used suitably.

The cosmetic of the present invention may be applied in various kinds of cosmetics. Illustrative examples thereof include a skin care product, a makeup product, a hair product, an antiperspirant product, and a UV-protection product. Particularly preferably, the cosmetic is used as an external application for a skin, such as a skin care cosmetic, a makeup cosmetic, an antiperspirant cosmetic, and a UV-protection cosmetic, and as an external application for a hair such as a hair cosmetic.

Illustrative examples of the skin care cosmetic include a beauty lotion, a milky lotion, a cream, a cleansing cream, a pack, an oil liquid, a massage material, a liquid cosmetic, a beauty oil, a cleaner, a deodorant, a hand cream, a lip cream, and a wrinkle concealer. Illustrative examples the makeup cosmetic include a makeup foundation, a concealer, a white powder, a powder foundation, a liquid foundation, a cream foundation, an oil foundation, a rouge, an eye color, an eye shadow, a mascara, an eye liner, an eye blow, and a lipstick. Illustrative examples of the antiperspirant cosmetic include a roll-on type, a cream type, a solution type, and a stick type. Illustrative examples of the UV-protection cosmetic include a sunscreen oil, a sunscreen lotion, and a sunscreen cream. Illustrative examples of the hair cosmetic include a shampoo, a rinse, a treatment, and a setting material.

The cosmetic of the present invention may be used in any of the following configurations; powder, oil liquid, water-in-oil emulsion, oil-in-water emulsion, non-aqueous emulsion, multi-emulsion such as W/O/W and O/W/O, and so on. In addition, form of the cosmetic of the present invention may be selected from various forms including a liquid form, a milky liquid form, a cream form, a solid form, a paste form, a gel form, a powder form, a pressed form, a multilayer form, a mousse form, a spray form, a stick form, and a pencil form.

Examples

Hereinafter, the present invention will be explained specifically by showing Preparation Example, Examples, and Comparative Examples; but the present invention is not limited to the following Examples. Meanwhile, in these Examples, a dynamic viscosity was measured with a capillary viscometer at 25 degrees C, and "%" used in concentration and content means "% by mass".

<Preparation Example>
(Preparation of an aqueous disperse solution of a silicone elastomer)
Into a 1-L glass beaker were taken 400 g of a methyl vinyl polysiloxane having a dynamic viscosity of 4900 mm²/second as shown by the following formula (4) and 7 g of a methyl hydrogen polysiloxane having a dynamic viscosity of 30 mm²/second as shown by the following formula (5) (blending ratio of the hydrosilyl group to the vinyl group is 1.1 to 1), and they were mixed and dissolved by using a homomixer. Thereafter, 33 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.) and 35 g of water were added thereinto; and then, when the resulting mixture was agitated by using a homomixer, viscosity thereof was increased to the state in which agitation was no more possible. The thickened mixture thus resulted was kneaded with a homodisper for 15 minutes. Then, 523 g of water was added thereinto and the resulting mixture was mixed by using a homomixer, resulting in obtaining a white, homogeneous emulsion. This emulsion was transferred to a 1-L glass flask equipped with an agitator having an anchor blade; and after the temperature thereof was adjusted at 15 to 20 degrees C, a dissolved mixture solution comprising 0.6 g of a toluene solution of a chloroplatinic acid-olefin complex (Pt content of 0.5%) and 1.2 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.) was added thereinto; and then, the resulting mixture was agitated for 24 hours at the same temperature to obtain an aqueous disperse solution of a silicone elastomer.

Chemical formula 2

The volume-average particle diameter of the silicone elastomer thus obtained was measured to be 280 nm with a particle size distribution measurement instrument of a laser diffraction/scattering type (LA-920; manufactured by HORIBA, Ltd.). A methyl vinyl polysiloxane having a dynamic viscosity of 4900 mm²/second as shown by the formula (4), a methyl hydrogen polysiloxane having a dynamic viscosity of 30 mm²/second as shown by the formula (5), and a toluene solution of a chloroplatinic acid-olefin complex (Pt content of 0.5%) were mixed with the foregoing mixing ratio; and then, the resulting mixture was poured into an aluminum petri dish so as to give the depth of 10 mm, allowed to stand at 25 degrees C for 6 hours, and then heated in a constant temperature oven controlled at 50 degrees C for one hour. The cured product thus obtained was an unsticky rubber elastic body having hardness of 20 as measured with a durometer A hardness meter.

<Example 1>
(Production 1 of composite particle)
Into a 3-L glass flask, equipped with an agitator having an anchor blade and containing a mixed aqueous disperse solution comprising 120 g of talc particles (trade name of JA-69R with a plate-like morphology having average particle diameter of 10 um; manufactured by Asada Milling Co., Ltd.), 41 g (this amount corresponds to 14 parts by mass of the silicone elastomer relative to 100 parts by mass of the talc particles) of the aqueous disperse solution of the silicone elastomer obtained in the above preparation example, and 1280 g of water were added 0.33 g (this amount corresponds to 0.01 part by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) and 30 g of a 28% aqueous ammonia solution. At this point of time, pH of the solution was 11.5. After the temperature of the resulting mixture was adjusted at 5 to 10 degrees C, 29 g (this amount corresponds to 85 parts by mass of the silicone resin after the hydrolysis-condensation reaction relative to 100 parts by mass of the silicone elastomer) of methyl trimethoxy silane was gradually added thereinto over 20 minutes; and then, agitation was further continued for one hour while maintaining the solution temperature at 5 to 10 degrees C. Then, the temperature thereof was increased to 55 to 60 degrees C; and then, agitation was continued for one hour while maintaining the same temperature to complete the hydrolysis-condensation reaction of methyl trimethoxy silane. The suspended solution thus obtained was dehydrated by a filter press. The dehydrated matter was transferred to a 3-L glass flask equipped with an agitator having an anchor blade, and then 1000 g of water was added thereinto; after agitation was continued for 30 minutes, dehydration was done by using a filter press. The dehydrated matter was transferred again to the glass flask and then dried with agitation by immersing the flask in an oil bath heated at 110 degrees C to obtain free-flowing particles.

When the particle thus obtained was observed with an electron microscope, it was found that spherical particles having the size of about 300 nm were adhered uniformly onto surface of the plate-like particle thereby confirming a composite particle having the silicone elastomer adhered on surface of the talc particle (FIG. 1). In addition, it was found that the silicone elastomer was adhered onto the talc particle by using the resinous silicone as a binder. In other words, if there is no binder to adhere the silicone elastomer onto surface of the talc particle, it is assumed that the silicone elastomer may be removed from surface of the talc particle by a procedure such as rinsing with water and drying even if the silicone elastomer is adhered to surface of the talc particle. If the silicone elastomer is removed therefrom, it is assumed that, because the silicone elastomer has a high agglomeration tendency, particles thereof may be agglomerated with each other; but a particle having this sort of morphology was not observed with an electron microscope.

Further, 20 g of sodium bromide, 0.5 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.), 80 g of water, and 5 g of the composite particles were weighed into a 100-mL glass bottle; and then, the glass bottle was shaken for 30 minutes and then allowed to stand for 24 hours to observe floating and sedimentation of the particles. If the silicone elastomer were removed from surface of the talc particle, the silicone elastomer would have floated up because its specific gravity is smaller than sodium bromide; but entirety thereof was settled out. This result also suggests that the silicone elastomer is adhered to the talc particle by the silicone resin as a binder.

<Example 2>
(Production 2 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 0.32 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 42% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of Merquat 100 with average molecular weight of 150,000; manufactured by Nalco Japan Co., Ltd.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.

When the particle thus obtained was observed with an electron microscope, it was found that spherical particles having the size of about 300 nm were adhered uniformly onto surface of the plate-like particle thereby confirming a composite particle having the silicone elastomer adhered on surface of the talc particle. In addition, it was found that the silicone elastomer was adhered onto the talc particle by using the resinous silicone as a binder.

Further, 20 g of sodium bromide, 0.5 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.), 80 g of water, and 5 g of the composite particles were weighed into a 100-mL glass bottle; and then, the glass bottle was shaken for 30 minutes and then allowed to stand for 24 hours to observe floating and sedimentation of the particles. If the silicone elastomer were removed from surface of the talc particle, the silicone elastomer would have floated up because its specific gravity is smaller than sodium bromide; but entirety thereof was settled out. This result suggests that the silicone elastomer is adhered to the talc particle by the silicone resin as a binder.

<Example 3>
(Production 3 of composite particle)
Into a 3-L glass flask, equipped with an agitator having an anchor blade and containing a mixed aqueous disperse solution comprising 120 g of mica particles (trade name of Y-2300X with a plate-like morphology having average particle diameter of 19 um; manufactured by YAMAGUCHI MICA Co., Ltd.), 39 g (this amount corresponds to 13 parts by mass of the silicone elastomer relative to 100 parts by mass of the mica particles) of the aqueous disperse solution of the silicone elastomer obtained in the above preparation example, and 1284 g of water were added 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) and 30 g of a 28% aqueous ammonia solution. At this point of time, pH of the solution was 11.4. After the temperature of the resulting mixture was adjusted at 5 to 10 degrees C, 27 g of methyl trimethoxy silane (this amount corresponds to 85 parts by mass of the silicone resin after the hydrolysis-condensation reaction relative to 100 parts by mass of the silicone elastomer) was gradually added thereinto over 20 minutes; and then, agitation was further continued for one hour while maintaining the solution temperature at 5 to 10 degrees C. Then, the temperature thereof was increased to 55 to 60 degrees C; and then, agitation was continued for one hour while maintaining the same temperature to complete the hydrolysis-condensation reaction of methyl trimethoxy silane. The suspended solution thus obtained was dehydrated by a filter press. The dehydrated matter was transferred to a 3-L glass flask equipped with an agitator having an anchor blade, and then 1000 g of water was added thereinto; after agitation was continued for 30 minutes, dehydration was done by using a filter press. The dehydrated matter was transferred again to the glass flask and then dried with agitation by immersing the flask in an oil bath heated at 110 degrees C to obtain free-flowing particles.

When the particle thus obtained was observed with an electron microscope, it was found that spherical particles having the size of about 300 nm were adhered uniformly onto surface of the plate-like particle thereby confirming a composite particle having the silicone elastomer adhered on surface of the mica particle. In addition, it was found that the silicone elastomer was adhered onto the mica particle by using the resinous silicone as a binder.

Further, 20 g of sodium bromide, 0.5 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.), 80 g of water, and 5 g of the composite particles were weighed into a 100-mL glass bottle; and then, the glass bottle was shaken for 30 minutes and then allowed to stand for 24 hours to observe floating and sedimentation of the particles. If the silicone elastomer were removed from surface of the mica particle, the silicone elastomer would have floated up because its specific gravity is smaller than sodium bromide; but entirety thereof was settled out. This result suggests that the silicone elastomer is adhered to the mica particle by the silicone resin as a binder.

<Example 4>
(Production 4 of composite particle)
Into a 3-L glass flask, equipped with an agitator having an anchor blade and containing a mixed aqueous disperse solution comprising 120 g of sericite particles (trade name of SANSHIN MICA FSE with a plate-like morphology having average particle diameter of 10 um; manufactured by Sanshin Mining Ind. Co., Ltd.), 41 g (this amount corresponds to 14 parts by mass of the silicone elastomer relative to 100 parts by mass of the sericite particles) of the aqueous disperse solution of the silicone elastomer obtained in the above preparation example, and 1281 g of water were added 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) and 30 g of a 28% aqueous ammonia solution. At this point of time, pH of the solution was 11.4. After the temperature of the resulting mixture was adjusted at 5 to 10 degrees C, 28 g of methyl trimethoxy silane (this amount corresponds to 85 parts by mass of the silicone resin after the hydrolysis-condensation reaction relative to 100 parts by mass of the silicone elastomer) was gradually added thereinto over 20 minutes; and then, agitation was further continued for one hour while maintaining the solution temperature at 5 to 10 degrees C. Then, the temperature thereof was increased to 55 to 60 degrees C; and then, agitation was continued for one hour while maintaining the same temperature to complete the hydrolysis-condensation reaction of methyl trimethoxy silane. The suspended solution thus obtained was dehydrated by a filter press. The dehydrated matter was transferred to a 3-L glass flask equipped with an agitator having an anchor blade, and then 1000 g of water was added thereinto; after agitation was continued for 30 minutes, dehydration was done by using a filter press. The dehydrated matter was transferred again to the glass flask and then dried with agitation by immersing the flask in an oil bath heated at 110 degrees C to obtain free-flowing particles.

When the particle thus obtained was observed with an electron microscope, it was found that spherical particles having the size of about 300 nm were adhered uniformly onto surface of the plate-like particle thereby confirming a composite particle having the silicone elastomer adhered on surface of the sericite particle. In addition, it was found that the silicone elastomer was adhered onto the sericite particle by using the silicone resin as a binder.

Further, 20 g of sodium bromide, 0.5 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.), 80 g of water, and 5 g of the composite particles were weighed into a 100-mL glass bottle; and then, the glass bottle was shaken for 30 minutes and then allowed to stand for 24 hours to observe floating and sedimentation of the particles. If the silicone elastomer were removed from surface of the sericite particle, the silicone elastomer would have floated up because its specific gravity is smaller than sodium bromide; but entirety thereof was settled out. This result suggests that the silicone elastomer is adhered to the sericite particle by the silicone resin as a binder.

<Example 5>
(Production 5 of composite particle)
Into a 3-L glass flask, which was equipped with an agitation equipment having an anchor blade and contained therein an aqueous mixed disperse solution of 150 g of mica titanium particle (trade name of Flamenco Red 420C having a plate-like form with particle diameter of 6 to 48 um, manufactured by BASF SE), 31 g of the aqueous silicone elastomer disperse solution obtained by the preparation example as mentioned above (this amount corresponds to 8 parts by mass of the silicone elastomer relative to 100 parts by mass of mica titanium), and 1261 g of water, were charged 0.33 g of a 40% aqueous solution of dimethyl dially ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000, manufactured by TOHO Chemical Industry Co., Ltd.; this amount corresponds to 0.01 part by mass relative to 100 parts by mass of water) and 30 g of a 28% aqueous ammonia. The pH of the solution at this time was 11.4. After temperature thereof was adjusted at 5 to 10 degrees C, 28 g of methyl trimethoxy silane (this amount corresponds to 109 parts by mass of a silicone resin after the hydrolysis-condensation reaction relative to 100 parts by mass of the silicone elastomer) was gradually added thereinto over 20 minutes with keeping temperature of the solution at 5 to 10 degrees C; and then, agitation of the solution was further continued for one hour. Then, the solution was heated to 55 to 60 degrees C; and then, the solution was agitated for one hour with keeping this temperature to complete the hydrolysis-condensation reaction of methyl trimethoxy silane. The suspension solution thus obtained was dehydrated by using a filter press. The dehydrated matter was transferred to a 3-L glass flask equipped with an agitation equipment having an anchor blade, and then added thereinto with 1000 g of water; and the resulting mixture was agitated for 30 minutes, and then dehydrated by a filter press. The dehydrated matter was transferred again to a glass flask and then dried with agitation while keeping the flask in an oil bath at 110 degrees C to obtain a free-flowing particle.

Observation of the obtained particle with an electron microscope revealed that spherical particles having a size of about 300 nm were uniformly adhered onto surface of the plate-like particle, so that it was confirmed that a composite particle having the silicone elastomer adhered onto surface of the mica titanium was formed. It was also found that the silicone elastomer was adhered onto mica titanium by using a silicone resin as a binder.

Further, 20 g of sodium bromide, 0.5 g of polyoxyethylene lauryl ether (trade name of Emulgen 109P; manufactured by Kao Corp.), 80 g of water, and 5 g of the composite particles were weighed into a 100-mL glass bottle; and then, the glass bottle was shaken for 30 minutes and then allowed to stand for 24 hours to observe floating and sedimentation of the particles. If the silicone elastomer were removed from surface of the mica titanium particle, the silicone elastomer would have floated up because its specific gravity is smaller than aqueous sodium bromide; but entirety thereof was settled out. This result also suggests that the silicone elastomer is adhered onto the mica titanium particle by the silicone resin as a binder.

<Comparative Example 1>
(Production 6 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1 was not added.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered to surface of the plate-like particle, the amount thereof was small, while agglomerate of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established (FIG. 2).

<Comparative Example 2>
(Production 7 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 0.13 g of sodium polyacrylate (trade name of Aqualic IH; anionic water-soluble polymer manufactured by Nippon Shokubai Co., Ltd.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered to surface of the plate-like particle, the amount thereof was small, while agglomerate of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established.

<Comparative Example 3>
(Production 8 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 0.44 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 30% aqueous solution of dodecyl trimethyl ammonium chloride (trade name of Cation BB; manufactured by NOF Corp.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.
When the particle thus obtained was observed with an electron microscope, similarly to Comparative Example 1, although there were spherical particles adhered to surface of the plate-like particle, the amount thereof was small, while agglomerate of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established.

<Comparative Example 4>
(Production 9 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 4.4 g (this amount corresponds to 0.1 parts by mass relative to 100 parts by mass of water) of a 30% aqueous solution of dodecyl trimethyl ammonium chloride (trade name of Cation BB; manufactured by NOF Corp.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered to surface of the plate-like particle, approximately half of the particles was adhered in the state of agglomerate; and thus, the desired adhesion state could not be established.

<Comparative Example 5>
(Production 10 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 0.13 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of sodium lauryl sulfate (trade name of Nikkol SLS; manufactured by Nikko Chemicals Co., Ltd.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.
When the particle thus obtained was observed with an electron microscope, similarly to Comparative Example 1, although there were spherical particles adhered to surface of the plate-like particle, the amount thereof was small, while agglomerate of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established.

<Comparative Example 6>
(Production 11 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 1 except that 1.3 g (this amount corresponds to 0.1 parts by mass relative to 100 parts by mass of water) of sodium lauryl sulfate (trade name of Nikkol SLS; manufactured by Nikko Chemicals Co., Ltd.) was used instead of 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 1.
When the particle thus obtained was observed with an electron microscope, agglomerate of the spherical particles were found, but spherical particles adhered to surface of the plate-like particle were not found at all.

<Comparative Example 7>
(Production 12 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 3 except that 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000, manufactured by Toho Chemical Industry Co., Ltd.) in Example 3 was not added.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered to surface of the plate-like particle, the amount thereof was small, while agglomerate of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established.

<Comparative Example 8>
(Production 13 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 4 except that 0.33 g (this amount corresponds to 0.01 parts by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000, manufactured by Toho Chemical Industry Co., Ltd.) in Example 4 was not added.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered to the plate-like particle surface, the adherence thereof was inhomogeneous because particles of much adhered as well as less adhered were present; and thus, the desired adhesion state could not be established.

<Comparative Example 9>
(Production 14 of composite particle)
A free-flowing particle was obtained in a manner similar to that in Example 5 except that 0.33 g (this amount corresponds to 0.01 part by mass relative to 100 parts by mass of water) of a 40% aqueous solution of dimethyl diallyl ammonium chloride polymer (trade name of ME Polymer H40W with average molecular weight of 240,000; manufactured by Toho Chemical Industry Co., Ltd.) in Example 5 was not added.
When the particle thus obtained was observed with an electron microscope, although there were spherical particles adhered onto surface of the plate-like particle, the amount thereof was small, while agglomerates of the spherical particles which were not adhered thereonto were found; and thus, the desired adhesion state could not be established.

<Characteristic evaluation in cosmetic uses>
Each of the composite particles obtained in Examples 1, 3, and 5, and Comparative Examples 1, 7, and 9 was evaluated by 10 expert panelists as to spreading property (extendability), softness (use feeling), adhesion (adhesivity and uniformity), powder dispersibility, and corrective effect of a skin figure (soft focus effect) at the time of application of a simple powder mixture according to the following prescription (Examples 6 to 8 and Comparative Examples 10 to 12). The results of them are shown in Table 2.

<Prescription>
Simple powder mixture
Composite particle of the foregoing Example or Comparative Example: 4 parts
Untreated talc: 92 parts
Dimethyl polysiloxane (6 mm²/2-seconds (25 degrees C)): 2 parts
Squalane: 2 parts
Total: 100 parts

Example 6
This is a simple mixture containing the composite particle of Example 1.
Example 7
This is a simple mixture containing the composite particle of Example 3.
Example 8
This is a simple mixture containing the composite particle of Example 5.
Comparative Example 10
This is a simple mixture containing the composite particle of Comparative Example 1.
Comparative Example 11
This is a simple mixture containing the composite particle of Comparative Example 7.
Comparative Example 12
This is a simple mixture containing the composite particle of Comparative Example 9.

<Preparation method>
In the prescription for the simple powder mixture, respective powder portions (the untreated talc and the composite particle in the foregoing Examples and Comparative Examples) were weighed and agitated by a high-speed blender for one minute. The oil portions (dimethyl polysiloxane and squalane) were added thereinto; and then, after the resulting mixture was agitated for 6 minutes, the mixture was passed through a 100-mesh filter to obtain a simple powder mixture or a simple powder mixture blank.

<Evaluation>
Spreading property (extendability), softness (use feeling), adhesion (adhesivity and uniformity), powder mixing (dispersibility), and corrective effect of a skin figure (soft focus effect) at the time of application of the simple powder mixture were evaluated in accordance with the evaluation criteria shown in Table 1. The respective results were judged in accordance with the following judgment criteria based on the average score of 10 peoples (Table 2).

<Judgment criteria>
Average score of 4.5 or more: Excellent
Average score of 3.5 or more and less than 4.5: Good
Average score of 2.5 or more and less than 3.5: Fair
Average score of 1.5 or more and less than 2.5: Poor
Average score of less than 1.5: Bad

As can be seen in Table 2, it was demonstrated that the cosmetics according to the present invention (Examples 6 to 8) have good usability such as spreading property (extendability), softness (use feeling), and adhesion (adhesivity and uniformity), good powder mixing property (dispersibility), and excellent corrective effect of a skin figure (soft focus effect), as compared with the cosmetics of Comparative Examples 10 to 12.

Examples 9 to 10 and Comparative Example 13
<Powder foundation>
In the following Examples, powder foundation was prepared by using powders of the composite particles obtained by the foregoing Example 1 or 4 with the composition ratio shown in Table 3.

(note 1) Treatment with methylhydrogen polysiloxane: 95 parts of talc used in Example 1 or sericite used in Example 4 was taken into a reactor, into which was gradually added with agitation 5 parts of methylhydrogen polysiloxane diluted in toluene. Temperature was increased to distill out toluene; and then, baking treatment was done with agitation at 150 degrees C for 3 hours to obtain talc which was treated with methylhydrogen polysiloxane and sericite which was treated with methylhydrogen polysiloxane, respectively.
(note 2) Polymethyl silsesquioxane: KMP-590 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation of cosmetic>
Ingredients 4 to 14 were charged into a Henschel mixer; and then, they were agitated and mixed. Into this were added ingredients 1 to 3 which were uniformly dissolved separately; and then, agitation and mixing were continued further. Into this was further added ingredient 15. The mixture thereby obtained was crushed by a hammer mill and press-molded in an appropriate aluminum pan to obtain a powder foundation. The powder foundation thus obtained was evaluated as to the items shown below. Meanwhile, in Comparative Example 13, none of ingredients 5 and 10 were blended thereinto.

<Use evaluation>
Evaluation was done, in accordance with the criteria shown in Table 4, by 10 women expert panelists on the powder foundation thus obtained as to spreading property (extendability), softness (use feeling), adhesion (adhesivity and uniformity), and corrective effect of a skin figure (soft focus effect) at the time of application of the cosmetic test sample, whereby spreading property (extendability), softness (use feeling), and adhesion (adhesivity and uniformity) at the time of application of the cosmetic, as well as natural makeup feeling of the cosmetic (bare skin feeling) and cosmetic durability (sustainability) were evaluated.

<Evaluation criteria>
Spreading property (extendability), softness (use feeling), and adhesion (adhesivity and uniformity) at the time of application of the cosmetic test sample, as well as natural makeup feeling of the cosmetic (bare skin feeling) and cosmetic durability (sustainability) were evaluated in accordance with the criteria shown in Table 4; and the average score obtained was judged by the following criteria. The results are shown in Table 5.

As can be seen in Table 5, Examples 9 and 10 show good usability, natural makeup feeling, and good cosmetic durability as compared with Comparative Example 13; and thus, it was demonstrated that these were excellent powder foundations.

Example 11
<Oil-in-water cream>
(Ingredients) mass (%)
1. Crosslinking dimethyl polysiloxane (note 1): 10.0
2. Glyceryl trioctanoate: 5.0
3. Composite powder of Example 5 (mica titanium): 1.0
4. Dipropylene glycol: 7.0
5. Glycerin: 5.0
6. Methyl cellulose (2% aqueous solution) (note 2): 7.0
7. Polyacrylamide emulsifier (note 3): 2.0
8. Preservative: appropriate amount
9. Fragrance: appropriate amount
10. Purified water: remainder
Total: 100.0
(note 1) Crosslinking dimethyl polysiloxane: KSG-16 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Methyl cellulose: Metolose SM-4000 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Polyacrylamide emulsifier: Sepigel 305 (manufactured by SEPIC S. A.)

<Preparation method>
A: Ingredients 4 to 10 were mixed.
B: Ingredients 1 to 3 were mixed, and then, they were added into A; the resulting mixture was emulsified by agitation.

The oil-in-water cream thus obtained was highly fine while having wide and light spreading properties without stickiness and greasiness, and yet having a soft use feeling and a corrective effect of a skin figure; and in addition, good cosmetic durability and excellent stability to temperature change and time passage could be confirmed.

Example 12
<Emulsified cream foundation>
(Ingredients) mass (%)
1. Alkyl-modified crosslinking polyether-modified silicone (note 1): 2.0
2. Alkyl-modified crosslinking dimethyl polysiloxane (note 2): 2.0
3. Liquid paraffin: 2.0
4. Trioctanoin: 5.0
5. Isotridecyl isononanoate: 9.0
6. Silicone co-modified with alkyl and polyether (note 3): 1.5
7. Hybrid silicone composite powder (note 4): 2.0
8. Composite powder of Example 3 (mica): 1.0
9. Iron oxide treated with triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone (note 5): 2.5
10. Titanium oxide treated with triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone (note 5): 7.5
11. 1,3-Butylene glycol: 5.0
12. Sodium citrate: 3.0
13. Magnesium sulfate: 3.0
14. Preservative: appropriate amount
15. Fragrance: appropriate amount
16. Purified water: remainder
Total: 100.0
(note 1) Alkyl-modified crosslinking polyether-modified silicone: KSG-310 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Alkyl-modified crosslinking dimethyl polysiloxane: KSG-41 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Silicone co-modified with alkyl and polyether: KF-6038 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 4) Hybrid silicone composite powder: KSP-100 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 5) Triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 6 were mixed uniformly, and then, ingredients 7 to 10 were added thereinto uniformly.
B: Ingredients 11 to 14 and 16 were dissolved.
C: With agitation, B was added gradually into A and they were emulsified; after cooling thereof, ingredient 15 was added thereinto to obtain the emulsified cream foundation.

The emulsified cream foundation thus obtained was low viscous and highly fine while having wide and light spreading properties without stickiness and greasiness, and yet having a soft use feeling and a corrective effect of a skin figure; and in addition, good cosmetic durability and excellent stability to temperature change and time passage could be confirmed.

Example 13
<Water-in-oil cream>
(Ingredients) mass (%)
1. Alkyl-modified crosslinking polyether-modified silicone (note 1): 6.0
2. Alkyl-modified crosslinking dimethyl polysiloxane (note 2): 2.0
3. Liquid paraffin: 13.5
4. Macademia nut oil: 5.0
5. Silicone co-modified with alkyl and polyether (note 3): 1.0
6. Hybrid silicone composite powder (note 4): 2.0
7. Composite powder of Example 3 (mica): 1.0
8. Sodium citrate: 0.2
9. Dipropylene glycol: 8.0
10. Glycerin: 3.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0
(note 1) Alkyl-modified crosslinking polyether-modified silicone: KSG-310 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Alkyl-modified crosslinking dimethyl polysiloxane: KSG-41 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Silicone co-modified with alkyl and polyether: KF-6038 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 4) Hybrid silicone composite powder: KSP-100 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 7 were mixed.
B: Ingredients 8 to 13 were mixed and dissolved, and then added into A for emulsification by agitation to obtain the water-in-oil cream.

The water-in-oil cream thus obtained was highly fine while having wide and light spreading properties without stickiness and greasiness, and yet having a soft use feeling and a corrective effect of a skin figure; and in addition, good cosmetic durability and excellent stability to temperature change and time passage could be confirmed.

Example 14
<Water-in-oil cream>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 16.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 4.0
3. Polyether-modified silicone (note 1): 5.0
4. POE (5) octyl dodecyl ether: 1.0
5. Polyoxyethylene sorbitan monostearate (20 E. O.): 0.5
6. Composite powder of Example 5 (mica titanium): 2.0
7. Plate-like barium sulfate (note 2): 2.0
8. Liquid paraffin: 2.0
9. Macadamia nut oil: 1.0
10. Scutellaria root extract (note 3): 1.0
11. Gentian extract (note 4): 0.5
12. Ethanol: 5.0
13. 1,3-Butylene glycol: 2.0
14. Preservative: appropriate amount
15. Fragrance: appropriate amount
16. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Plate-like barium sulfate: HL (manufactured by Sakai Chemical Industry Co., Ltd.)
(note 3) Scutellaria root extract: extracted by a 50% aqueous 1,3-butylene glycol solution
(note 4) Gentian extract: extracted by a 20% aqueous ethanol solution

<Preparation method>
A: Ingredients 6 to 9 were mixed and dispersed uniformly.
B: Ingredients 1 to 5 were mixed, and then, A was added thereinto.
C: After ingredients 10 to 14 and 16 were mixed, B was added thereinto to form an emulsion.
D: Ingredient 15 was added into C to obtain the water-in-oil cream.

The water-in-oil cream thus obtained was highly fine while having wide and light spreading properties without stickiness, and yet having excellent adhesion, a soft use feeling, and a corrective effect of a skin figure; and in addition, it had excellent cosmetic durability. Because there was no change by temperature change and time passage, excellent stability could be confirmed.

Example 15
<Eye liner>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 39.0
2. Polyether-modified silicone (note 1): 3.0
3. Organic silicone resin (note 2): 15.0
4. Montomorillonite modified with dioctadecyl dimethyl ammonium salt: 3.0
5. Black iron oxide treated with methylhydrogen polysiloxane: 8.0
6. Composite powder of Example 3 (mica): 2.0
7. 1,3-Butylene glycol: 5.0
8. Sodium dehydroacetate: appropriate amount
9. Preservative: appropriate amount
10. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Organic silicone resin: KF-7312J (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 4 were mixed, and then ingredients 5 and 6 were added thereinto; the resulting mixture was dispersed uniformly.
B: Ingredients 7 to 10 were mixed.
C: B was added gradually into A; and then, they were emulsified to obtain the eye liner.

The eye liner thus obtained had light spreading property and thus was easy to draw; and in addition, it had a clean and fresh use feeling without stickiness. It was excellent in usability and stability without any change by temperature and passage of time; and in addition, it was confirmed that the eye liner was excellent not only in water-resistance and perspiration-resistance property but also in cosmetic durability.

Example 16
<Foundation>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 45.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 5.0
3. Polyether-modified branched silicone (note 1): 3.5
4. Montomorillonite modified with octadecyl dimethyl benzyl ammonium salt: 1.5
5. Composite powder of Example 3 (mica): 2.0
6. Iron oxide treated with triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone (note 2): 2.5
7. Titanium oxide treated with triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone (note 2): 7.5
8. Dipropylene glycol: 5.0
9. Methyl para-oxybenzoate ester: 0.3
10. Fragrance: appropriate amount
11. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified branched silicone: KF-6028 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Triethoxy silyl ethyl polydimethylsiloxyethyl hexyl dimethicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 4 were mixed with heating; and then, ingredients 5 to 7 were added thereinto so as to be uniform.
B: Ingredients 8 to 9 and 11 were dissolved.
C: With agitation, B was added gradually into A to form an emulsion; after cooling thereof, ingredient 10 was added thereinto to obtain the foundation.

The foundation thus obtained was highly fine while having wide and light spreading properties without stickiness and greasiness, and yet having a soft use feeling and a corrective effect of a skin figure; in addition, good cosmetic durability and excellent stability to temperature change and time passage could be confirmed.

Example 17
<Eye shadow>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 17.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 10.0
3. Polyether-modified branched silicone (note 1): 2.0
4. PEG (10) lauryl ether: 0.5
5. Composite powder of Example 3 (mica): 2.0
6. Composite powder of Example 1 (talc): 1.0
7. Composite powder of Example 5 (mica titanium): 6.0
8. Inorganic color pigment treated with methylhydrogen polysiloxane: appropriate amount
9. Sodium chloride: 2.0
10. Propylene glycol: 8.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified branched silicone: KF-6028 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 4 were mixed, and then ingredients 5 to 8 were added thereinto; and then, they were dispersed uniformly.
B: Ingredients 9 to 11 and 13 were dissolved uniformly.
C: B was gradually added into A with agitation for emulsification; and then, ingredient 12 was added thereinto to obtain the eye shadow.

The eye shadow thus obtained had wide and light spreading properties and a soft use feeling without greasiness and powderiness. In addition, it was excellent in water-resistance, water-repellency, perspiration-resistance, and durability without cosmetic deterioration. Excellent stability could be confirmed because there was no change with time passage and temperature change.

Example 18
<Lipstick>
(Ingredients) mass (%)
1. Candellila wax: 7.0
2. Polyethylene wax: 8.0
3. Acryl silicone resin having a long-chain alkyl (note 1): 12.0
4. Methyl phenyl polysiloxane (note 2): 3.0
5. Isotridecyl isononanoate: 20.0
6. Glyceryl isostearate: 16.0
7. Polyglyceryl triisostearate: 28.5
8. Composite powder of Example 3 (mica): 0.5
9. Composite powder of Example 5 (mica titanium): 5.0
10. Organic pigment: appropriate amount
11. Fragrance: appropriate amount
Total: 100.0
(note 1) Acryl silicone resin having a long chain alkyl: KP-561P (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Methyl phenyl polysiloxane: KF-54 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 6 and a part of ingredient 7 were dissolved by mixing and heating.
B: Ingredients 8 to 10 and the rest of ingredient 7 were mixed uniformly; and then, they were added into A to make them uniform.
C: Ingredient 11 was added into B to obtain the lipstick.

The lipstick thus obtained had a light spreading property and a soft use feeling without greasiness and powderiness; in addition, it was excellent in water-resistance, water-repellency, durability, and stability.

Example 19
<Lipstick>
(Ingredients) mass (%)
1. Polyethylene: 7.0
2. Microcrystalline wax: 3.0
3. Acryl silicone resin having a long-chain alkyl (note 1): 10.5
4. Triethyl hexanoin: 19.5
5. Neopentyl glycol diethyl hexanoate: 15.0
6. Neopentyl glycol dicaprylate: 7.0
7. Hydrogenated polyisobutene: 2.5
8. Methyl phenyl polysiloxane (note 2): 7.5
9. Diglyceryl triisostearate: 0.8
10. Composite powder of Example 5 (mica titanium): 6.0
11. Color pigment: appropriate amount
12. Fragrance: appropriate amount
Total: 100.0
(note 1) Acryl silicone resin having a long-chain alkyl: KP-561P (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Methyl phenyl polysiloxane: KF-54HV (viscosity: 5850 cs, manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 8 were dissolved by heating and mixing.
B: Ingredients 9 and 11 were uniformly mixed and then added into A so as to make them uniform.
C: Ingredients 10 and 12 were added into B; and then, they were mixed uniformly to obtain the lipstick.

The lipstick thus obtained had a light spreading property without greasiness and powderiness while being shiny and having a soft use feeling; in addition, it was excellent in water-resistance, water-repellency, durability, and stability.

Example 20
<Eye liner>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 6.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 5.0
3. Jojoba oil: 2.0
4. Polyether-modified silicone (note 1): 1.0
5. Silicone co-modified with alkyl and polyether (note 2): 1.0
6. Acryl silicone resin (note 3): 15.0
7. Composite powder of Example 3 (mica): 2.0
8. Black iron oxide treated with methylhydrogen polysiloxane: 18.0
9. Ethanol: 5.0
10. Preservative: appropriate amount
11. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Silicone co-modified with alkyl and polyether: KF-6038 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Acryl silicone resin: KP-545 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 6 were mixed by agitation; and then, ingredients 7 and 8 were added thereinto so as to disperse them uniformly.
B: Ingredients 9 to 11 were dissolved by agitation.
C: With agitation, B was added gradually into A; and then, they were emulsified to obtain the eye liner.

The eye liner thus obtained had a light spreading property and a soft use feeling without greasiness and powderiness; in addition, it was excellent in water-resistance, water-repellency, perspiration-resistance and durability without cosmetic deterioration. It showed excellent stability because there was no change with time passage and temperature change.

Example 21
<Liquid milky foundation>
(Ingredients) mass (%)
1. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 4.5
2. Decamethyl cyclopentasiloxane: 30.0
3. Squalane: 4.0
4. Neopentyl glycol dioctanoate: 3.0
5. Diglyceride triisostearate: 2.0
6. alpha-Monoisostearyl glyceryl ether: 1.0
7. Polyether-modified silicone (note 1): 1.0
8. Silicone co-modified with alkyl and polyether (note 2): 0.5
9. Aluminum distearate salt: 0.2
10. Composite powder of Example 4 (sericite): 2.0
11. Composite powder of Example 1 (talc): 1.0
12. Iron oxide pigment treated with methylhydrogen polysiloxane: appropriate amount
13. Glycerin: 3.0
14. Preservative: appropriate amount
15. Fragrance: appropriate amount
16. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Silicone co-modified with alkyl and polyether: KF-6038 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 9 were mixed with heating; and then, ingredients 10 to 12 were added thereinto so as to make them uniform.
B: Ingredients 13 to 14 and 16 were dissolved by heating.
C: With agitation, B was added gradually into A so as to make them emulsion; and after cooling thereof, ingredient 15 was added thereinto to obtain the liquid milky foundation.

The liquid milky foundation thus obtained was low viscous and highly fine while having wide and light spreading properties without stickiness and greasiness, and yet having a soft use feeling and a corrective effect of a skin figure; and in addition, good cosmetic durability and excellent stability to temperature change and time passage could be confirmed.

Example 22
<Liquid foundation>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 16.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 8.0
3. Octyl para-methoxycinnamate: 3.0
4. 12-hydroxystearic acid: 1.0
5. Fluorine-modified silicone (note 1): 15.0
6. Silicone co-modified with fluorinated alkyl and polyether (note 2): 5.0
7. Spherical polymethyl silsesquioxane powder (note 3): 1.0
8. Composite powder of Example 1 (talc): 1.0
9. Composite powder of Example 5 (mica titanium): 1.0
10. Iron oxide pigment treated with methylhydrogen polysiloxane: appropriate amount
11. Ethanol: 15.0
12. Glycerin: 3.0
13. Magnesium sulfate: 1.0
14. Preservative: appropriate amount
15. Fragrance: appropriate amount
16. Purified water: remainder
Total: 100.0
(note 1) Fluorine-modified silicone: FL-50 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Silicone co-modified with fluorinated alkyl and polyether: FPD-4694 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Spherical polymethyl silsesquioxane powder: KMP-590 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 7 to 10 were mixed uniformly.
B: Ingredients 1 to 6 were mixed with heating at 70 degrees C; and then, A was added thereinto and the resulting mixture was mixed and dispersed uniformly.
C: Ingredients 11 to 14 and 16 were heated at 40 degrees C, and then added gradually into B to form emulsion; after cooling thereof, ingredient 15 was added thereinto to obtain the liquid foundation.

The liquid foundation thus obtained had wide and light spreading properties without stickiness while having a soft use feeling and a corrective effect of a skin figure; and in addition, excellent stability to temperature change and time passage could be confirmed.

Example 23
<Eye liner>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 22.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 5.0
3. Black iron oxide treated with methylhydrogen polysiloxane: 20.0
4. Composite powder of Example 3 (mica): 1.0
5. Organic silicone resin (note 1): 10.0
6. Vitamin E acetate: 0.2
7. Jojoba oil: 2.0
8. Dimethyl distearyl ammonium hectorite: 3.0
9. Polyether-modified silicone (note 2): 2.0
10. Ethanol: 3.0
11. 1,3-Butylene glycol: 5.0
12. Preservative: appropriate amount
13. Purified water: remainder
Total: 100.0
(note 1) Organic silicone resin: KF-7312J (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 2 and 5 to 9 were mixed; and after ingredients 3 and 4 were added thereinto, the resulting mixture was mixed and dispersed uniformly.
B: Ingredients 10 to 13 were mixed.
C: B was added gradually into A; and then, they were emulsified to obtain the eye liner.

The eye liner thus obtained had light spreading property and thus was easy to draw; and in addition, it had a clean, fresh, and soft use feeling without stickiness. There was no change by temperature or passage of time; and in addition, it was confirmed that the eye liner was excellent not only in water-resistance and perspiration-resistance property but also in cosmetic durability.

Example 24
<Foundation>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 27.0
2. Methyl phenyl polysiloxane: 3.0
3. Neopentyl glycol dioctanoate: 10.0
4. Polyether-modified silicone (note 1): 4.0
5. Glyceryl trioctanoate: 3.0
6. Composite powder of Example 1 (talc): 1.0
7. Composite powder of Example 4 (sericite): 1.0
8. Composite powder of Example 5 (mica titanium): 2.0
9. Titanium oxide treated with aluminum stearate: 6.0
10. Iron oxide pigment treated with methylhydrogen polysiloxane: appropriate amount
11. 1,3-Butylene glycol: 7.0
12. Sodium chloride: 0.5
13. Preservative: appropriate amount
14. Fragrance: appropriate amount
15. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6017 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 5 were mixed and dissolved; and then, ingredients 6 to 10 were dispersed uniformly thereinto.
B: After ingredients 11 to 13 and 15 were mixed, they were added into A so as to make an emulsion.
C: Ingredient 14 was added into B to obtain the foundation.

The foundation thus obtained had wide and light spreading properties and excellent adhesion without stickiness, while having a soft use feeling and a corrective effect of a skin figure; and in addition, it had good cosmetic durability. In addition, excellent stability to temperature change and time passage could be confirmed.

Example 25
<Brushing material spray>
(Ingredients) mass (%)
1. Isopropyl myristate: 1.0
2. Stearyl trimethyl ammonium chloride: 0.05
3. Composite powder of Example 3 (mica): 0.5
4. Ethanol: 25.0
5. Fragrance: appropriate amount
6. Propellant: remainder
Total: 100.0

<Preparation method>
A: Ingredients 1 to 5 were mixed.
B: After A was charged into an aerosol can, and then ingredient 6 was filled thereinto to obtain the brushing material spray.

The brushing material spray thus obtained had very smooth use feeling and excellent durability; and in addition, it was confirmed that the material spray had good powder dispersibility during the time of its use and was easy combing and shinny.

Example 26
<Rinse>
(Ingredients) mass (%)
1. Ethylene glycol distearate: 3.0
2. Cetanol: 2.0
3. Propylene glycol monostearate: 3.0
4. Dimethyl polysiloxane (100 mm²/second (25 degrees C)): 3.0
5. Glycerin monostearate: 4.0
6. Polyoxyethylene (3) stearate: 4.0
7. Acetyl trimethyl ammonium chloride: 5.0
8. Polyoxyethylene (20) cetyl ether: 2.0
9. Composite powder of Example 3 (mica): 1.0
10. 1,3-Butylene glycol: 5.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0

<Preparation method>
A: Ingredients 1 to 9 were mixed by agitation.
B: Ingredients 10 to 11 and 13 were mixed with heating.
C: B was added into A; and after mixing and cooling of them, ingredient 12 was added thereinto to obtain the rinse.

The rinse thus obtained was neither sticky nor heavy during its use while giving a shiny look and a voluminous feeling to a hair with non-stickiness and smoothness; and in addition, good combing properties, usability, and durability could be confirmed.

Example 27
<Rinse in shampoo>
(Ingredients) mass (%)
1. Laurylamide propyldimethylaminoacetic acid betaine (30%): 15.0
2. Sodium polyoxyethylene (3) lauryl ether sulfate (27%): 4.0
3. Polyoxyethylene (150) distearate: 0.5
4. Cationic cellulose (4%): 0.5
5. Glycerin: 3.0
6. Dimethyl polysiloxane (1000000 mm²/second (25 degrees C)): 1.0
7. Dimethyl polysiloxane (100 mm²/second (25 degrees C)): 3.0
8. Composite powder of Example 3 (mica): 1.0
9. Preservative: appropriate amount
10. Fragrance: appropriate amount
11. Purified water: remainder
Total: 100.0

<Preparation method>
A: Ingredients 1 to 5, 9, and 11 were mixed with heating.
B: Ingredients 6 to 8 were mixed and dispersed.
C: B was added into A; and after mixing and cooling thereof, ingredient 10 was added thereinto to obtain the rinse in shampoo.

The rinse in shampoo thus obtained was neither sticky nor heavy during its use while giving a shiny look and a non-sticky, smooth, and voluminous feeling to a hair; and in addition, good combing properties, usability, and durability could be confirmed.

Example 28
<Treatment>
(Ingredients) mass (%)
1. Ethylene glycol distearate: 1.0
2. Liquid paraffin: 10.0
3. Squalane: 5.0
4. Stearyl alcohol: 1.5
5. Dimethyl polysiloxane (10 mm²/second (25 degrees C)): 3.0
6. Stearic acid: 6.0
7. Polyoxyethylene (3) stearyl alcohol: 4.5
8. Polyoxyethylene (150) cetyl ether: 2.0
9. Composite powder of Example 3 (mica): 1.0
10. 1,3-Butylene glycol: 6.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0

<Preparation method>
A: Ingredients 1 to 9 were mixed with heating.
B: Ingredients 10 to 11 and 13 were mixed and dispersed.
C: B was added into A; and after mixing and cooling thereof, ingredient 12 was added thereinto to obtain the treatment.

The treatment thus obtained was neither sticky nor heavy during its use while giving a shiny look and a non-sticky, smooth, and voluminous feeling to a hair; and in addition, good combing properties, usability, and durability could be confirmed.

Example 29
<Water-in-oil type antiperspirant>
(Ingredients) mass (%)
1. Crosslinking polyether-modified silicone (note 1): 7.0
2. Decamethyl cyclopentasiloxane: 13.0
3. Glyceryl trioctanoate: 7.0
4. Dipropylene glycol: 5.0
5. Sodium citrate: 0.2
6. Aluminum-zirconium tetrachloro hydrate: 18.0
7. Composite powder of Example 1 (talc): 2.0
8. Fluorine-modified hybrid silicone composite powder (note 2): 2.0
9. Fragrance: appropriate amount
10. Purified water: remainder
Total: 100.0
(note 1) Crosslinking polyether-modified silicone: KSG-210 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Fluorine-modified hybrid silicone composite powder: KSP-200 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 3 were mixed.
B: Ingredients 4 to 10 were mixed.
C: B was added into A; and they were mixed and emulsified to obtain the water-in-oil type antiperspirant.

The water-in-oil type antiperspirant thus obtained had a light spreading property without stickiness and greasiness; and in addition, it had excellent usability and stability to temperature change and time passage.

Example 30
<Roll-on type antiperspirant>
(Ingredients) mass (%)
1. Crosslinking polyether-modified silicone (note 1): 20.0
2. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 10.0
3. Crosslinking dimethyl polysiloxane (note 2): 15.0
4. Decamethyl cyclopentasiloxane: 30.0
5. Aluminum-zirconium tetrachloro hydrate: 20.0
6. Composite powder of Example 3 (mica): 5.0
7. Fragrance: appropriate amount
Total: 100.0
(note 1) Crosslinking polyether-modified silicone: KSG-210 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Crosslinking dimethyl polysiloxane: KSG-15 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 4 were mixed.
B: Ingredients 5 to 7 were added into A; and the resulting mixture was uniformly dispersed to obtain the roll-on type antiperspirant.

The roll-on type antiperspirant thus obtained had a light spreading property without stickiness and greasiness; in addition, it was excellent in usability and stability without change by temperature and time passage.

Example 31
<Sunscreen milky lotion>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 20.0
2. Methyl phenyl polysiloxane: 3.0
3. Sorbitan monoisostearate: 1.0
4. Polyether-modified silicone (note 1): 0.5
5. Trimethyl siloxy silicate (note 2): 1.0
6. Octyl para-methoxycinnamate: 4.0
7. Composite powder of Example 5 (mica titanium): 1.0
8. Titanium oxide microparticle treated with aluminum stearate: 6.0
9. Sorbitol: 2.0
10. Sodium chloride: 2.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0
(note 1) Polyether-modified silicone: KF-6015 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Trimethyl siloxy silicate: X-21-5250 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 6 were mixed with heating; and then, ingredients 7 and 8 were dispersed uniformly thereinto.
B: Ingredients 9 to 11 and 13 were mixed with heating.
C: With agitation, B was added gradually into B so as to make an emulsion; and after cooling thereof, ingredient 12 was added thereinto to obtain the sunscreen milky lotion.

The sunscreen milky lotion thus obtained was highly fine while having wide and light spreading properties without stickiness, and yet having a soft use feeling and a corrective effect of a skin figure. In addition, it had good cosmetic durability thereby having sustainable UV-protection effect; and in addition, excellent stability was confirmed without any change by temperature change and time passage.

Example 32
<Sun-cut cream>
(Ingredients) mass (%)
1. Decamethyl cyclopentasiloxane: 20.0
2. Acryl silicone resin (note 1): 12.0
3. Glyceryl trioctanoate: 5.0
4. Octyl para-methoxycinnamate: 6.0
5. Crosslinking polyether-modified silicone (note 2): 5.0
6. Silicone co-modified with alkyl-silicone and polyether (note 3): 6.5
7. Composite powder of Example 5 (mica titanium): 1.0
8. Titanium oxide microparticle treated with aluminum stearate: 15.0
9. Sodium chloride: 0.5
10. 1,3-Butylene glycol: 2.0
11. Preservative: appropriate amount
12. Fragrance: appropriate amount
13. Purified water: remainder
Total: 100.0
(note 1) Acryl silicone resin: KP-545 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Crosslinking polyether-modified silicone: KSG-210 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Silicone co-modified with alkyl-silicone and polyether: KF-6038 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredient 2 was added into a part of ingredient 1 so as to be uniform, and then, ingredient 8 was added thereinto; the resulting mixture was dispersed by a bead mill.
B: The rest of ingredient 1 and ingredients 3 to 7 were mixed uniformly.
C: Ingredients 9 to 11 and 13 were mixed and dissolved.
D: C was added into B so as to make an emulsion, and then, A was dispersed thereinto; ingredient 12 was further added thereinto to obtain the sun-cut cream.

The sun-cut cream thus obtained had wide and light spreading properties and excellent adhesion without stickiness, while having a soft use feeling and a corrective effect of a skin figure; and in addition, it had good cosmetic durability. In addition, excellent stability to temperature change and time passage could be confirmed.

Example 33
<Nail enamel>
(Ingredients) mass (%)
1. Acryl silicone resin (note 1): 45.0
2. Methyl trimethicone (note 2): 5.0
3. Nitrocellulose: 3.0
4. Camphor: 0.5
5. Acetyltributyl citrate: 1.0
6. Dimethyl distearyl ammonium hectorite: 0.5
7. Butyl acetate: 30.0
8. Ethyl acetate: 10.0
9. Isopropyl alcohol: 5.0
10. Composite powder of Example 3 (mica):
appropriate amount
Total: 100.0
(note 1) Acryl silicone resin: KP-549 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Methyl trimethicone:TMF-1.5 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 7 to 9 were mixed; and then, ingredients 4 to 6 were added thereinto and the resulting mixture was mixed uniformly.
B: Ingredients 1 to 3 were added into A; and then, they were mixed.
C: Ingredient 10 was added into B; and then, they were mixed to obtain the nail enamel.

The nail enamel thus obtained had wide and light spreading properties, a smooth look, and good durability because of good oil-resistance and water-resistance, while not having an oppressing feeling to nails and not yellowing of nails; and in addition, excellent stability was confirmed because there was no change in a cosmetic film by temperature change and time passage.

Example 34
<Cheek color>
(Ingredients) mass (%)
1. Crosslinking dimethyl polysiloxane (note 1): 28.0
2. Decamethyl cyclopentasiloxane: 34.5
3. Neopentyl glycol dioctanoate: 9.0
4. Stearoyl inulin: 10.0
5. Hybrid silicone composite powder (note 2): 2.0
6. Red No. 202: appropriate amount
7. Iron oxide treated with alkyl-silicone branch type silicone (note 3): appropriate amount
8. Titanium oxide treated with alkyl-silicone branch type silicone (note 3): appropriate amount
9. Tocopherol: appropriate amount
10. Composite powder of Example 5 (mica titanium): 5.0
11. Composite powder of Example 3 (mica): 11.5
Total: 100.0
(note 1) Crosslinking dimethyl polysiloxane: KSG-16 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Hybrid silicone composite powder: KSP-100 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Alkyl-silicone branch type silicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 5 were mixed, and then heated to 80 degrees C so as to make uniform dispersion.
B: Ingredients 6 to 11 were added into A; and then, the resulting mixture was dispersed uniformly at 80 degrees C.
C: By cooling to room temperature, the cheek color was obtained.

The cheek color thus obtained was in the form of a sponge so that it could be readily taken out, and had wide and light spreading properties and a use feeling without greasiness and powderiness. The cheek color had good water-resistance, water-repellent and perspiration-resistance properties, and durability without cosmetic deterioration; and in addition, excellent stabilities to temperature change and time passaged could be confirmed.

Example 35
<Eye color>
(Ingredients) mass (%)
1. Isotridecyl isononanoate: 20.0
2. Squalane: 20.0
3. Hybrid silicone composite powder (note 1): 6.0
4. Dextrin palmitate: 10.0
5. Crosslinking dimethyl polysiloxane (note 2): 12.0
6. Barium sulfate: 5.0
7. Polyethylene terephthalate/Al powder: 4.5
8. Composite powder of Example 5 (mica titanium): 13.5
9. Tocopherol: appropriate amount
10. Glass flake powder for cosmetic (note 3): 1.5
11. Glass flake powder for cosmetic covered with
iron oxide (note 4): 7.5
Total: 100.0
(note 1) Hybrid silicone composite powder: KSP-100 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Crosslinking dimethyl polysiloxane: KSG-16 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Glass flake (manufactured by Nippon Sheet Glass Co., Ltd.)
(note 4) Glass flake covered with iron oxide: Metashine (manufactured by Nippon Sheet Glass Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 5 were mixed and heated to 90 degrees C so as to make uniform dispersion.
B: Ingredients 6 to 11 were added into A; and then, the resulting mixture was dispersed uniformly at 90 degrees C.
C: The mixture was cooled to room temperature to obtain the eye color.

The eye color thus obtained was in the form of a jerry so that it could be readily taken out, and it had wide and light spreading properties and a use feeling without greasiness and powderiness. The eye color had good water-resistance, water-repellent and perspiration-resistance properties, and durability without cosmetic deterioration; and in addition, excellent stabilities to temperature change and time passaged could be confirmed.

Example 36
<Foundation>
(Ingredients) mass (%)
1. Dimethyl polysiloxane (6 mm²/second (25 degrees C)): 23.0
2. Organic silicone resin (note 1): 10.0
3. Alkyl-silicone branch-crosslinking dimethyl polysiloxane (note 2): 34.0
4. Hybrid silicone composite powder (note 3): 8.0
5. Squalane: 1.0
6. Jojoba oil: 1.0
7. Diphenyl siloxyphenyl trimethicone (note 4): 1.0
8. PMMA spherical powder: 2.0
9. Iron oxide treated with alkyl-silicone branch type silicone (note 5): appropriate amount
10. Titanium oxide treated with alkyl-silicone branch type silicone (note 5): 6.0
11. Titanium oxide microparticle treated with aluminum stearate: 9.0
12. Tocopherol: appropriate amount
13. Composite powder of Example 1 (talc): 3.0
14. Composite powder of Example 4 (sericite): 2.0
Total: 100.0
(note 1) Organic silicone resin: KF-7312L (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Alkyl-silicone branch-crosslinking dimethyl polysiloxane: KSG-048Z (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Hybrid silicone composite powder: KSP-105 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 4) Diphenyl siloxyphenyl trimethicone: KF-56A (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 5) Alkyl-silicone branch type silicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: A part of ingredient 1 and ingredients 2 to 8 were mixed and dispersed uniformly.
B: Ingredients 9 to 14 and the rest of ingredient 1 were uniformly dispersed by a roll mill.
C: B was uniformly dispersed in A to obtain the foundation.

The foundation thus obtained was in the form of a souffle so that it could be readily taken out, and it had wide and light spreading properties and a use feeling without greasiness and powderiness. The foundation had good water-resistance, water-repellent and perspiration-resistance properties, and durability without cosmetic deterioration; and in addition, excellent stabilities to temperature change and time passaged could be confirmed.

Example 37
<Eye color>
(Ingredients) mass (%)
1. Dimethyl polysiloxane (20 mm²/second (25 degrees C)): 1.0
2. Diphenyl siloxyphenyl trimethicone (note 1): 1.0
3. Squalane: 1.5
4. Vaseline: 2.5
5. Spherical polymethyl silsesquioxane powder (note 2): 2.0
6. PMMA spherical powder: 1.0
7. Zinc myristate: 8.0
8. Fumed silica: 0.5
9. Iron oxide treated with alkyl-silicone branch type silicone (note 3): appropriate amount
10. Ultramarine blue treated with alkyl-silicone branch type silicone (note 3): appropriate amount
11. Titanium oxide treated with alkyl-silicone branch type silicone (note 3): appropriate amount
12. Tocopherol: appropriate amount
13. Composite powder of Example 1 (talc): 20.0
14. Composite powder of Example 3 (mica): 10.0
15. Composite powder of Example 4 (sericite): 10.0
16. Composite powder of Example 5 (mica titanium): 25.0
Total: 100.0
(note 1) Diphenyl siloxyphenyl trimethicone:KF-56A (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Spherical polymethyl silsesquioxane powder: KMP-590 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Alkyl-silicone branch type silicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 5 to 16 were mixed by agitation in a Henschel mixer.
B: Ingredients 1 to 4 were uniformly dispersed and then added into A; the resulting mixture was mixed by agitation.
C: The mixture was crushed by a hammer mill and then press-molded in an appropriate aluminum pan to obtain the eye color.

The eye color thus obtained could be readily taken out, and had wide and light spreading properties and a use feeling without greasiness and powderiness. The eye color had good water-resistance, water-repellent and perspiration-resistance properties, and durability without cosmetic deterioration; and in addition, excellent stabilities to temperature change and time passaged could be confirmed.

Example 38
<Eye color>
(Ingredients) mass (%)
1. Isododecane: 17.0
2. Acryl silicone resin (note 1): 20.0
3. Acryl silicone resin having a long-chain alkyl (note 2): 2.0
4. Hybrid silicone composite powder (note 3): 6.0
5. Vaseline: 10.0
6. Alkyl-modified crosslinking dimethyl polysiloxane (note 4): 12.0
7. Barium sulfate: 5.0
8. Organic pigment: appropriate amount
9. Iron oxide treated with alkyl-silicone branch type silicone (note 5): appropriate amount
10. Titanium oxide treated with alkyl-silicone branch type silicone (note 5): appropriate amount
11. Composite powder of Example 5 (mica titanium): 20.0
12. Tocopherol: appropriate amount
13. Fragrance: appropriate amount
Total: 100.0
(note 1) Acryl silicone resin: KP-550 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 2) Acryl silicone resin having a long-chain alkyl: KP-561P (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 3) Hybrid silicone composite powder: KSP-441 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 4) Alkyl-modified crosslinking dimethyl polysiloxane: KSG-42 (manufactured by Shin-Etsu Chemical Co., Ltd.)
(note 5) Alkyl-silicone branch type silicone: KF-9909 (manufactured by Shin-Etsu Chemical Co., Ltd.)

<Preparation method>
A: Ingredients 1 to 6 were mixed and dispersed uniformly.
B: Ingredients 7 to 13 were added into A; and then, the resulting mixture was uniformly dispersed to obtain the eye color.

It is to be noted that the present invention is not limited to the above embodiments. The above embodiments are merely illustrative, and whatever having the substantially same configurations as the technical concept recited in the appended claims and exhibiting the same functions and effects are embraced within the technical scope of the present invention.

Claims

A method for producing a composite particle, wherein a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them is added into a mixed solution obtained by blending, at least, a mixed aqueous disperse solution in which an inorganic powder and a silicone elastomer are dispersed, a cationic water-soluble polymer, and an alkaline substance, whereby carrying out a hydrolysis-condensation reaction to produce a composite particle formed of the inorganic powder whose surface is adhered with the silicone elastomer by using a silicone resin as a binder.
The method for producing a composite particle according to claim 1, wherein the cationic water-soluble polymer is synthetic, not containing an anionic and an amphoteric group, obtained by synthesizing a polymer skeleton thereof with any of a vinyl polymerization, an addition polymerization, and a condensation.
The method for producing a composite particle according to claim 2, wherein the cationic water-soluble polymer synthesized without using a monomer having a nonionic group is used.
The method for producing a composite particle according to claim 3, wherein a polymer of dimethyl diallyl ammonium chloride is used as the cationic water-soluble polymer.
The method for producing a composite particle according to any one of claims 1 to 4, wherein adding amount of the cationic water-soluble polymer to the mixed aqueous disperse solution is 0.0001 to 1 part by mass relative to 100 parts by mass of water in the mixed aqueous disperse solution.
A method for producing a cosmetic, wherein the cosmetic is produced by using the composite particle produced by the method for producing a composite particle according to any one of claims 1 to 5.
A cosmetic, wherein the cosmetic contains a composite particle produced by a hydrolysis-condensation reaction of a compound selected from an alkoxy silane, a silanol group-containing silane, and a partial condensate of them added into a mixed solution containing a cationic water-soluble polymer, an alkaline substance, and an aqueous mixture disperse solution in which an inorganic powder and a silicone elastomer are dispersed, thereby forming the composite particle having the silicone elastomer adhered onto surface of the inorganic powder by using a silicone resin as a binder.
The cosmetic according to claim 7, wherein the composite particle is produced by using the cationic water-soluble polymer which is a synthetic polymer whose polymer skeleton, containing neither an anionic group nor an amphoteric group, is synthesized by any of a vinyl polymerization, an addition polymerization, and a condensation.
The cosmetic according to claim 8, wherein the composite particle is produced by using the cationic water-soluble polymer which is synthesized by not using a monomer having a nonionic group.
The cosmetic according to claim 9, wherein the composite particle is produced by using a polymer of dimethyl diallyl ammonium chloride as the cationic water-soluble polymer.
The cosmetic according to any one of claims 7 to 10, wherein the composite particle is produced by using the cationic water-soluble polymer with the amount thereof against the aqueous mixture disperse solution being in the range of 0.0001 to 1 parts by mass relative to 100 parts by mass of water in the aqueous mixture disperse solution.