HK1130275B - Inorganic-organic nanocomposite - Google Patents

Description

Inorganic-organic nanocomposite

Technical Field

The present invention relates generally to improved nanocomposite compositions and methods of making and using the same. More particularly, the present invention relates to inorganic-organic nanocomposites and methods for their preparation. The invention also relates to the use of these inorganic-organic nanocomposite compositions in, for example, coatings, sealants, caulks, adhesives and plastics.

Background

Inorganic-organic nanocomposites may exhibit mechanical properties that are superior to their individual components. In order to optimize the properties of these materials, it is often desirable to disperse the inorganic components in the organic matrix on a nanometer length scale. Clays and other layered inorganic materials that can be broken into nanoscale building blocks can be used to prepare inorganic-organic nanocomposites.

The addition of clay materials to polymers is known in the art, however, the incorporation of clay into polymers may not provide the desired improvement in the physical, especially mechanical, properties of the polymer. This may be due to, for example, a lack of affinity at the interface of the clay and polymer or at the boundary of the clay and polymer within the material. By dispersing the clay material uniformly throughout the polymer, the affinity between the clay and the polymer can improve the physical properties of the resulting nanocomposite. The relatively large surface area of the clay, if uniformly dispersed, can provide more interfaces between the clay and the polymer, and can subsequently improve physical properties by reducing the mobility of the polymer chains at these interfaces. Conversely, in the absence of affinity between the clay and the polymer, the strength and uniformity of the composition can be negatively affected by having a concentrated clay cluster (pocket) rather than being uniformly dispersed throughout the polymer. The affinity between clay and polymer is related to the fact that: clays are generally hydrophilic in nature, while polymers are generally hydrophobic.

The clay mineral is typically made of fine particlesAnd has a platy crystalline (platy) aluminum silicate. The crystal structure of a typical clay mineral is formed by reaction with AlO (OH)₂Octahedrally connected SiO₄A multilayer structure composed of a combination of tetrahedral layers. Clay minerals vary based on the combination of their constituent layers and cations. Isomorphous substitution of cations of clay minerals, e.g. Al, usually occurs³⁺Or Fe³⁺By substitution of Si in tetrahedral networks⁴⁺Ions, or Al³⁺、Mg²⁺Or Fe²⁺Replacing other cations within the octahedral network, and imparting a net negative charge to the clay structure. Naturally occurring elements within the clay gallery (galley), such as water molecules or sodium or potassium ions, are absorbed onto the surface of the clay layers due to this net negative charge.

To promote greater affinity of the clay and polymer at the interface and provide uniform dispersion of the clay within the polymer, the interlayer surface chemistry of the clay may be modified such that the silicate layers are less hydrophilic.

Alkylammonium ions, such as onium salts, are commonly used to prepare clay dispersions for nanocomposites. The basic formula of a typical alkylammonium ion is CH₃-(CH₂)_n-NH₃ ⁺Wherein n is 1 to 18. It is believed that alkylammonium ions also readily exchange with naturally occurring cations present in the clay platelets (platelets), thereby creating intercalated states. In addition, it is believed that alkylammonium ions can increase the spacing between clay layers and can also reduce the surface energy of the clay, allowing organic species having different polarities to be inserted between clay layers.

There remains a need for nanocomposites with improved properties. The invention disclosed herein provides a cost-effective and efficient method to produce novel inorganic-organic nanocomposite compositions that are particularly suitable for use in sealants where the desired softness, processability and elasticity characteristics are important performance criteria.

Summary of The Invention

According to the present invention, there is provided an inorganic-organic nanocomposite material comprising at least one inorganic component and at least one organic component, said inorganic component being layered inorganic nanoparticles and said organic component being a quaternary ammonium organopolysiloxane.

The novel inorganic-organic nanocomposites of the present invention are useful as fillers in a wide variety of polymer resin-containing compositions, and in particular as fillers in such compositions, intended for uses such as sealants, coatings and adhesives.

Detailed Description

According to the present invention, there is provided an inorganic-organic nanocomposite material comprising at least one inorganic component and at least one organic component, said inorganic component being layered inorganic nanoparticles and said organic component being a quaternary ammonium organopolysiloxane. When describing the present invention, the following terms have the following meanings, unless otherwise specified.

Definition of

The term "exfoliation" as used herein describes a process in which small packets of nanoclay platelets are separated from each other in a polymer matrix. During exfoliation, the platelets in the outermost region of each packet cleave, exposing more platelets for separation.

The term "gallery (galley)" as used herein describes the space between parallel layers of clay platelets. The gallery space varies depending on the nature of the molecule or polymer occupying the space. The interlayer spacing between individual nanoclay platelets also varies depending on the type of molecule occupying the space.

The term "intercalant" as used herein includes any inorganic or organic compound that is capable of entering the clay gallery and bonding to its surface.

The term "intercalate" as used herein refers to a clay-chemical complex in which the clay gallery space is increased due to a surface modification process. Under appropriate temperature and shear conditions, the insert can flake off in the resin matrix.

The term "intercalation" as used herein refers to the process of forming an insert.

The expression "inorganic nanoparticles" as used herein describes layered inorganic materials, such as clays, in which one or more dimensions (e.g., length, width, or thickness) are in the nanometer size range and are capable of ion exchange.

The expression "modified clay" as used herein refers to a clay material, such as a nanoclay, treated with any inorganic or organic compound capable of undergoing ion exchange reactions with cations present at the interlayer surfaces of the clay.

The term "nanoclay" as used herein describes a clay material having a unique morphology wherein one dimension is in the nanometer range. Nanoclays can form chemical complexes with intercalants ionically associated with the surfaces between the layers making up the clay particles. This association of the intercalant and clay particles results in a material that is compatible with many different types of matrix resins (host resins) to disperse the clay filler therein.

The term "nanoparticle" as used herein refers to a particle size generally less than about 1000nm, which is generally determined by diameter.

The term "platelet" as used herein refers to a single layer of a layered material.

The inorganic nanoparticles in the inorganic-organic nanocomposite material can be natural or synthetic (e.g., smectite clay) and should have certain ion exchange properties, such as smectite clay, rectorite, vermiculite, illite, mica and synthetic analogs thereof, including synthetic clays, synthetic mica-montmorillonite and tetrasilicic mica.

In a first embodiment, the nanoparticles may have an average largest lateral dimension (width) of from about 0.01 μm to about 10 μm, in a second embodiment from about 0.05 μm to about 2 μm, and in a third embodiment from about 0.1 μm to about 1 μm. The average maximum longitudinal dimension (thickness) of the nanoparticles may generally vary from about 0.5nm to about 10nm in a first embodiment, and from about 1nm to about 5nm in a second embodiment.

Useful inorganic nanoparticle materials of the present invention include natural or synthetic phyllosilicates, particularly smectite clays such as montmorillonite, sodium montmorillonite, calcium montmorillonite, magnesium montmorillonite, nontronite, beidellite, volkonskoite, laponite, hectorite, saponite, sauconite, NaSiO, and the like₁₃(OH)₃.3H₂O (magadite), kenyaite, sobockite, svindordite, stevensite, talc, mica, kaolinite, vermiculite, halloysite, aluminate oxides or hydrotalcite, micaceous minerals such as illite and mixed layered illite/smectite minerals such as rectorite, tarosovite, ledikite and illite in admixture with one or more of the clay minerals described above. Any swellable layered material that sufficiently absorbs organic molecules to increase the interlayer spacing between adjacent phyllosilicate platelets to at least about 5 angstroms, or at least about 10 angstroms (when the phyllosilicate is measured dry), may be used to prepare the inorganic-organic nanocomposite of the invention.

The modified inorganic nanoparticles of the present invention are prepared by quantitatively providing exchangeable cations (e.g., Na)⁺、Ca²⁺、Al³⁺、Fe²⁺、Fe³⁺And Mg²⁺) Is contacted with at least one ammonium-containing organopolysiloxane. The resulting modified particles are inorganic-organic nanocomposites with intercalated organopolysiloxane ammonium ions.

The ammonium-containing organopolysiloxane must include at least one ammonium group and may include two or more ammonium groups. The quaternary ammonium groups may be located at the end of the organopolysiloxane and/or along the siloxane backbone. One class of useful ammonium-containing organopolysiloxanes has the general formula:

M_aD_bD′_c

wherein "a" is 2, "b" is equal to or greater than 1, and "c" is 0 or a positive number; m is

[R³ _zNR⁴]_3-x-yR¹ _xR² _ySiO_1/2

Wherein "x" is 0, 1 or 2 and "y" is 0 or 1, provided that x + y is less than or equal to 2, "z" is 2, R¹And R²Each independently a monovalent hydrocarbon group of up to 60 carbons; r³A monovalent hydrocarbon group selected from H and up to 60 carbons; r⁴Is a monovalent hydrocarbon group of up to 60 carbons; d is

R⁵R⁶SiO_1/2

Wherein R is⁵And R⁶Each independently a monovalent hydrocarbon group of up to 60 carbon atoms; and D' is

R⁷R⁸SiO_2/2

Wherein R is⁷And R⁸Each independently an amine-containing monovalent hydrocarbon group having the general formula:

[R⁹ _aNR¹⁰]

wherein "a" is 2, R⁹A monovalent hydrocarbon group selected from H and up to 60 carbons; r¹⁰Is a monovalent hydrocarbon group of up to 60 carbons.

In another embodiment of the present invention, the ammonium-containing organopolysiloxane is R¹¹R¹²R¹³N, wherein R¹¹、R¹²And R¹³Each independently an alkoxysilane or a monovalent hydrocarbon group of up to 60 carbons. The alkoxysilane has the general formula:

[R¹⁴O]_3-x-yR¹⁵ _xR¹⁶ _ySiR¹⁷

wherein "x" is 0, 1 or 2 and "y" is 0 or 1, provided that x + y is less than or equal to 2; r¹⁴Is at most 30A monovalent hydrocarbon group of carbon; r¹⁵And R¹⁶Each independently selected from monovalent hydrocarbon groups of up to 60 carbons; r¹⁷Is a monovalent hydrocarbon group of up to 60 carbons. Other compounds that may be used in the modified inorganic component of the present invention are amine compounds or compounds having the structure R¹⁸R¹⁹R²⁰N, wherein R is¹⁸、R¹⁹And R²⁰Each independently an alkyl or alkenyl group of up to 30 carbon atoms, and in another embodiment, each independently an alkyl or alkenyl group having up to 20 carbon atoms, which may be the same or different. In yet another embodiment, the organic molecule is a long chain tertiary amine, wherein R¹⁸、R¹⁹And R²⁰Each independently an alkyl or alkenyl group of 14 carbons to 20 carbons.

There is no need to convert the layered inorganic nanoparticle compositions of the present invention to a proton-exchanged form. Solvent and solventless processes are generally used. The organopolysiloxane ammonium ions are inserted into the layered inorganic nanoparticle material by cation exchange. In the solvent-based process, the organopolysiloxane ammonium component is placed in a solvent that is inert to the polymerization or coupling reaction. Particularly suitable solvents are water or water-polar cosolvent systems such as water-ethanol, water-acetone and the like. After removal of the solvent, an intercalated particulate concentrate is prepared. In solventless processes, a high shear blender is typically required to perform the intercalation reaction. The inorganic-organic nanocomposite material can be in the form of a suspension, gel, paste, or solid.

Specific types of ammonium-containing organopolysiloxanes are those described in U.S. patent 5,130,396, and can be prepared from known materials, including those commercially available, which is incorporated herein by reference.

The ammonium-containing organopolysiloxane of U.S. patent 5,130,396 is represented by the following general formula:

wherein R is¹And R²Identical or different and are represented by a group of formula:

wherein the nitrogen atom in (I) and the silicon atom in (II) are bonded through R⁵The radicals are linked, and R⁵Represents an alkylene group having 1 to 10 carbon atoms, a cycloalkylene group having 5 to 8 atoms or a unit of the general formula:

or

Wherein n is a number from 1 to 6 and denotes the number of methylene groups in the nitrogen position and m is a number from 0 to 6, as in the silica skeleton, the free valences of the oxygen atoms bound to the silicon atoms being saturated by silicon atoms of further radicals of the formula (II) and/or by metal atoms of one or more of the following cross-linking bonds

OrOrOr

Or

In which M is a silicon, titanium or zirconium atom and R' is a linear or branched alkyl radical having from 1 to 5 carbon atoms, and these radicals of the formula (II)Has a ratio of silicon atoms to metal atoms in the connecting bond of 1:0, and wherein R³Is equal to R¹Or R²Or hydrogen, or a linear or branched alkyl group having 1 to 20 carbon atoms, a cycloalkyl group having 5 to 8 carbon atoms or a benzyl group, and R⁴Equal to hydrogen, or a linear or branched alkyl group having from 1 to 20 carbon atoms, or a chloropropyl, cycloalkyl, benzyl, alkyl, propargyl, chloroethyl, or hydroxyethyl group consisting of from 5 to 8 carbon atoms, and X is an anion, X has a valence of 1 to 3 and is selected from the group consisting of halide, hypochlorite, sulfate, bisulfate, nitrite, nitrate, phosphate, dihydrogen phosphate, hydrogen phosphate, carbonate, bicarbonate, hydroxide, chlorate, perchlorate, chromate, dichromate, cyanide, cyanate, thiocyanate, sulfide, hydrogen sulfide, selenide, telluride, borate, metaborate, azide, tetrafluoroborate, tetraphenylborate, hexafluorophosphate, formate, acetate, propionate, oxalate, trifluoroacetate, trichloroacetate and benzoate.

The ammonium-containing organopolysiloxane compound described herein is in the form of macroscopically spherical particles having a diameter of 0.01 to 3.0mm and a specific surface area of 0 to 1000m²In terms of/g, a specific pore volume of 0 to 5.0ml/g, a bulk density of 50 to 1000g/l and a dry matter content relative to the volume of 50 to 750 g/l.

One method of preparing ammonium-containing organopolysiloxanes comprises reacting a primary, secondary or tertiary aminosilane having at least one hydrolyzable alkoxy group with water, optionally in the presence of a catalyst, to effect hydrolysis and subsequent silane condensation to produce an amine-terminated organopolysilane, which is subsequently quaternized with a suitable quaternizing reactant (e.g., an inorganic acid and/or an alkyl halide) to produce an ammonium-containing organopolysiloxane. This type of process is described in the aforementioned us patent 5,130,396. In this regard, U.S. patent 6,730,766, the entire contents of which are incorporated herein by reference, describes a method of making quaternized polysiloxanes by the reaction of epoxy-functional polysiloxanes.

In a variation of this method, a primary, secondary or tertiary aminosilane having a hydrolyzable alkoxy group is quaternized followed by a hydrolytic condensation reaction to provide an organopolysiloxane. For example, ammonium-containing N-trimethoxysilylpropyl-N, N, N-trimethylammonium chloride, N-trimethoxysilylpropyl-N, N, N-tri-N-butylammonium chloride and commercially available ammonium-containing trialkoxysilanoctadecyldimethyl (3-trimethoxysilylpropyl) ammonium chloride (available from Gelest, Inc.) provide the ammonium-containing organopolysiloxanes used herein after hydrolysis/condensation.

Other suitable tertiary aminosilanes that may be used to prepare the ammonium-containing organopolysiloxane include tris (triethoxysilylpropyl) amine, tris (trimethoxysilylpropyl) amine, tris (diethoxymethylsilylpropyl) amine, tris (tripropoxysilylpropyl) amine, tris (ethoxydimethylsilylpropyl) amine, tris (triethoxyphenylsilylpropyl) amine, and the like.

Another method of preparing ammonium-containing organopolysiloxanes requires quaternizing the primary, secondary or tertiary amine-containing organopolysiloxane using a quaternizing reactant. Useful amine-containing organopolysiloxanes include those of the general formula:

wherein R is¹、R²、R⁶And R⁷Each independently H, a hydrocarbyl group of up to 30 carbon atoms, e.g., alkyl, cycloalkyl, aryl, alkaryl, aralkyl, or the like, or R¹And R²Together or R⁶And R⁷Together form a divalent bridging group having up to 12 carbon atoms, R³And R⁵Each independently a divalent hydrocarbon bridging group having up to 30 carbon atoms, optionally containing one or more oxygen and/or nitrogen atoms in the chain, e.g. a straight or branched chain alkylene group having 1 to 8 carbon atoms, e.g. -CH₂-、-CH₂CH₂-、-CH₂CH₂CH₂-、-CH₂-C(CH₃)-CH₂-、-CH₂CH₂CH₂CH₂-etc. R⁴Each independently an alkyl group, and n is 1 to 20, and preferably 6 to 12.

These and similar amine-containing organopolysiloxanes can be prepared by known and conventional methods, for example by reacting an olefinic amine (e.g., allylamine) with a polydiorganosiloxane having Si-H bonds in the presence of a hydrosilation catalyst (e.g., a platinum-containing hydrosilation catalyst) as described in U.S. Pat. No. 5,026,890, the entire contents of which are incorporated herein by reference.

Specific amine-containing organopolysiloxanes useful in preparing the ammonium-containing organopolysiloxanes herein include the following technical mixtures:

and

the inorganic-organic nanocomposite material of the present invention is particularly useful as all or part of a filler in compositions containing solid polymers or mixtures/blends of solid polymers.

Useful solid polymers include epoxy resins, polycarbonates, silicones, polyesters, polyethers, polyolefins, natural and synthetic rubbers, polyurethanes, nylons, polystyrenes, polyvinylaromatic resins, acrylic resins, acrylate resins, polyamides, polyimides, phenolic resins, polyvinyl halides, polyphenylene oxides, polyketones, copolymers and blends thereof. Copolymers include both random and block copolymers. Polyolefin resins include polybutylene, polypropylene and polyethylene, such as low density polyethylene, medium density polyethylene, high density polyethylene and ethylene copolymers; polyvinyl halide resins include polyvinyl chloride polymers and copolymers, and polyvinylidene chloride polymers and copolymers, fluoropolymers; polyvinyl aromatic resins include polystyrene polymers and copolymers; acrylate resins include polymers and copolymers of acrylates and methacrylates, polyamide resins include nylon 6, nylon 11, and nylon 12, and polyamide copolymers and blends thereof, polyester resins include polyalkylene terephthalates, such as polyethylene terephthalate and polybutylene terephthalate, and polyester copolymers; synthetic rubbers include styrene-butadiene and acrylonitrile-butadiene-styrene copolymers; and polyketones include polyetherketones and polyetheretherketones.

In the resin-filled composition of the present invention, the inorganic-organic nanocomposite is, of course, present in an amount to enhance gas barrier properties. In a first embodiment, the inorganic-organic nanocomposite may be present in an amount up to about 90 weight percent, in a second embodiment in an amount up to about 50 weight percent, and in a third embodiment in an amount up to about 20 weight percent.

The inorganic-organic nanocomposite of the present invention is also preferably used as a filler in compositions intended to act as a gas barrier, for example in compositions disclosed and claimed in a pending application entitled "room temperature curable organopolysiloxane composition" filed by the applicant on the same day, the content of which is incorporated herein in its entirety.

The invention is illustrated by the following non-limiting examples:

example 1

The inorganic-organic nanocomposite of the present invention was prepared as follows: 10g of aminopropyl terminated siloxane ("GAP 10", siloxane length 10, from GE Silicones, Waterford, USA) was first placed in a 100ml single neck round bottom flask and 4ml of methanol (from Merck) was added. 2.2ml of concentrated hydrochloric acid are added very slowly with stirring. Stirring was continued for 10 minutes. 900ml of water was added to a 2000ml three-necked round bottom flask equipped with a condenser and an overhead mechanical stirrer. 18g of Cloisite Na are very slowly stirred (stirring rate about 250rpm)⁺(Natural MongolianDesliming, obtained from Southern Clayproducts) clay was added to the water. The ammonium chloride solution (prepared as above) was then added very slowly to the clay-water mixture. The mixture was stirred for 1 hour and left to stand overnight. The mixture was filtered through a Buckner funnel and the resulting solid was slurried with 800ml of methanol, stirred for 20 minutes, and the mixture was then filtered. The solid was dried in an oven at 80 ℃ for about 50 hours.

While the preferred embodiments of the invention have been illustrated and described in detail, various modifications, such as components, materials, and parameters, will be apparent to those skilled in the art, and it is intended to cover in the appended claims all such modifications and changes as fall within the scope of the invention.

Claims (22)

1. An inorganic-organic nanocomposite comprising at least one inorganic component that is a layered inorganic nanoparticle and at least one organic component that is a quaternary ammonium organopolysiloxane; wherein the layered inorganic nanoparticles have a particle size, as determined by diameter, of less than 1000nm and are capable of ion exchange; the quaternary ammonium organopolysiloxane is at least one ammonium-containing diorganopolysiloxane having the formula:

M_aD_bD′_c

wherein "a" is 2, "b" is equal to or greater than 1, and "c" is 0 or a positive number; m is

[R³ _zNR⁴]_3-x-yR¹ _xR² _ySiO_1/2

Wherein "x" is 0, 1 or 2, and "y" is 0 or 1, provided that x + y is less than or equal to 2, "z" is 2, R¹And R²Each independently a monovalent hydrocarbon group of up to 60 carbons; r³A monovalent hydrocarbon group selected from H and up to 60 carbons; r⁴Is a monovalent hydrocarbon group of up to 60 carbons; d is

R⁵R⁶SiO_1/2

Wherein R is⁵And R⁶Each independently a monovalent hydrocarbon group of up to 60 carbon atoms; and D' is

R⁷R⁸SiO_2/2

Wherein R is⁷And R⁸Each independently an amine-containing monovalent hydrocarbon group having the general formula:

[R⁹ _aR¹⁰]

wherein "a" is 2, R⁹A monovalent hydrocarbon group selected from H and up to 60 carbons; r¹⁰Is a monovalent hydrocarbon group of up to 60 carbons.

2. The inorganic-organic nanocomposite of claim 1, wherein the layered inorganic nanoparticles have exchangeable cations selected from Na⁺、Ca²⁺、Al³⁺、Fe²⁺、Fe³⁺、Mg²⁺And mixtures thereof.

3. The inorganic-organic nanocomposite of claim 1, wherein the layered nanoparticles are at least one selected from the group consisting of: montmorillonite, sodium montmorillonite, calcium montmorillonite, magnesium montmorillonite, nontronite, beidellite, volkonskoite, laponite, hectorite, saponite, sauconite, kenyaite, stevensite, vermiculite, halloysite, aluminate oxides, hydrotalcite, illite, rectorite, ledikite, kaolinite, and mixtures thereof.

4. The inorganic-organic nanocomposite of claim 1, wherein the layered inorganic nanoparticles have an average largest transverse dimension of from 0.01 microns to 10 microns and an average largest longitudinal dimension of from 0.5 nanometers to 10 nanometers.

5. The inorganic-organic nanocomposite of claim 1 wherein the quaternary ammonium group is of the formula R⁶R⁷R⁸N⁺X^-Is represented by the formula (I) in which R⁶、R⁷And R⁸At least one of which is an alkoxysilane having up to 60 carbon atoms and the remainder is an alkyl or alkenyl group having up to 60 carbon atoms, and X is an anion.

6. The inorganic-organic nanocomposite of claim 1, wherein the quaternary ammonium organopolysiloxane is obtained by: an aminosilane having at least one hydrolyzable group is reacted with water under hydrolysis/condensation conditions to provide an amine-terminated organopolysiloxane, and the amine-terminated organopolysiloxane is then quaternized to provide an ammonium organopolysiloxane.

7. The inorganic-organic nanocomposite of claim 1, wherein the quaternary ammonium organopolysiloxane is obtained by: the aminosilane having at least one hydrolyzable alkoxy group is quaternized prior to hydrolysis/condensation to provide an ammonium organopolysiloxane.

8. The inorganic-organic nanocomposite of claim 1, wherein the quaternary ammonium organopolysiloxane is obtained by: the amine-terminated organopolysiloxane is provided by hydrosilating the organopolysiloxane terminated with allylamine in the presence of a hydrosilation catalyst to provide an amine-terminated organopolysiloxane, followed by quaternizing the amine-terminated organopolysiloxane to provide an ammonium organopolysiloxane.

9. A method of preparing an inorganic-organic nanocomposite material, the method comprising the steps of:

a) reacting an aminosilane having at least one hydrolyzable alkoxy group with water, optionally in the presence of a catalyst, to provide an amine-terminated organopolysiloxane;

b) quaternizing the amine-terminated organopolysiloxane to provide a quaternized organopolysiloxane; and

c) combining the quaternized organopolysiloxane with layered inorganic nanoparticles having exchangeable cations provides an inorganic-organic nanocomposite.

10. The method of claim 9, wherein the aminosilane is a primary, secondary or tertiary aminosilane having at least one hydrolyzable alkoxy group.

11. The process of claim 9 wherein the catalyst is selected from the group consisting of organometallic compounds, acids, bases, and mixtures thereof.

12. The method of claim 9, wherein the amine-terminated organopolysiloxane is quaternized with a mineral acid, an alkyl halide, or a mixture thereof.

13. An inorganic-organic nanocomposite obtained by the process of claim 9.

14. An inorganic-organic nanocomposite obtained by the process of claim 10.

15. An inorganic-organic nanocomposite obtained by the process of claim 11.

16. An inorganic-organic nanocomposite obtained by the process of claim 12.

17. A composition comprising at least one solid synthetic resin and, as part or all of the filler therefor, at least one inorganic-organic nanocomposite material according to claim 1.

18. The composition of claim 17, wherein the resin is at least one selected from the group consisting of: epoxy resins, polycarbonates, silicones, polyesters, polyethers, polyolefins, natural and synthetic rubbers, polyurethanes, nylons, polystyrenes, polyvinylaromatic resins, acrylic resins, acrylate resins, polyimides, phenolic resins, polyvinyl halides, polyphenylene oxides, polyketones, copolymers and blends thereof.

19. The composition of claim 17, wherein the inorganic-organic nanocomposite is present in an amount of up to 90 weight percent.

20. A composition comprising at least one solid synthetic resin and, as part or all of the filler therefor, at least one inorganic-organic nanocomposite obtained by the process of claim 9.

21. The composition of claim 20, wherein the resin is at least one of epoxy, polycarbonate, silicone, polyester, polyether, polyolefin, natural and synthetic rubber, polyurethane, nylon, polystyrene, polyvinyl aromatic, acrylic, acrylate, polyimide, phenolic, polyvinyl halide, polyphenylene oxide, polyketone, copolymers and blends thereof.

22. The composition of claim 20, wherein the inorganic-organic nanocomposite is present in an amount of up to 90 weight percent.