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WO1997014280A1 - Plaquettes pour circuit imprime a caracteristiques dielectriques ameliorees - Google Patents

Plaquettes pour circuit imprime a caracteristiques dielectriques ameliorees Download PDF

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Publication number
WO1997014280A1
WO1997014280A1 PCT/US1996/016400 US9616400W WO9714280A1 WO 1997014280 A1 WO1997014280 A1 WO 1997014280A1 US 9616400 W US9616400 W US 9616400W WO 9714280 A1 WO9714280 A1 WO 9714280A1
Authority
WO
WIPO (PCT)
Prior art keywords
particles
epoxy resin
core
laminate
glass fiber
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/US1996/016400
Other languages
English (en)
Inventor
Cheng-Wu Chu
Mark D. Holte
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Honeywell International Inc
Original Assignee
AlliedSignal Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by AlliedSignal Inc filed Critical AlliedSignal Inc
Priority to AU72646/96A priority Critical patent/AU7264696A/en
Publication of WO1997014280A1 publication Critical patent/WO1997014280A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • B32B5/28—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer impregnated with or embedded in a plastic substance
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/036—Multilayers with layers of different types
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0203—Fillers and particles
    • H05K2201/0206—Materials
    • H05K2201/0209—Inorganic, non-metallic particles
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0203—Fillers and particles
    • H05K2201/0206—Materials
    • H05K2201/0212—Resin particles

Definitions

  • the invention relates generally to the field of laminates such as are widely used to make printed circuit boards. More specifically, the invention relates to improved laminates which have lower dielectric properties relative to those made solely of epoxy resins.
  • FR-2 phenolic resin impregnated paper
  • FR-3 is a paper composite which has been 5 impregnated with epoxy resins rather than phenolic resins.
  • CEM-1 is a composite which is more expensive than the FR-2 and FR-3 materials, but which provides improved electrical and physical properties.
  • an epoxy resin is used to coat paper as in FR-3, but the core is covered with glass 0 fiber reinforced epoxy resin outer layers.
  • CEM-3 uses an epoxy resin impregnated non-woven glass fiber core with epoxy resin impregnated woven glass cloth outer layers. It is a higher cost product and is used in somewhat more demanding applications than is CEM-1.
  • the invention 5 comprises an improved CEM-3 laminate for use in high voltage applications, such as in television tuners.
  • the dielectric constant of a material relates to the resistance of that material to an applied voltage. It is defined as the capacitance of the capacitor having a material as a dielectric to the capacitance of a capacitor in which air is the dielectric. Typical values for CEM- 3 are given by Coombs to 5 be about 4.6. In other words, the capacitance of the composite is a factor of 4.6 times that of air.
  • the dissipation factor relates to the electrical power which can be lost through a material.
  • the invention is a method of adjusting the 0 dielectric constant and dissipation factor in printed circuit boards, which is accomplished by adding polymeric particles to the thermoset polymers used in the insulating substrates.
  • the polymeric particles preferably are core-shell particles in which a rubbery polymer core is surrounded by a harder polymer 5 shell.
  • the particles typically will represent up to 25 wt.% of the substrate, based on the resin content. Preferably, the particles will be about 5-20 wt.%.
  • a particularly preferred core-shell particle has a average diameter of about 0.05 to 5 ⁇ m and has a core comprising a butadiene polymer and a shell comprising 0 a methacrylate polymer.
  • the invention is a laminate used in printed circuit boards comprising an insulating substrate containing up to 25 wt.% of polymeric particles having an average diameter of about 0.05 to 5 ⁇ m.
  • the 5 particles preferably are core-shell particles, especially those having a core comprising a butadiene polymer and a shell comprising a methacrylate polymer.
  • the invention is a method of improving the Comparative Tracking Index of insulating substrates used in printed circuit
  • 3 Q boards comprising incorporating in such insulating substrates up to 25 wt.% of polymeric particles having an average diameter of about 0.05 to 30 ⁇ m.
  • inorganic filler particles also may be added to the insulating substrates.
  • Particularly use ul are talc and aluminum silicate.
  • a CEM- 3 laminate includes such core-shell j D particles and is made with an inner layer of non-woven glass fiber reinforced epoxy resin and covering layers of woven glass fiber reinforced epoxy resin.
  • An alternative embodiment places the woven glass fiber resin in the center, -with covering layers of non-woven glass fiber.
  • Inorganic particles such as clays, talc, etc. typically are less expensive than epoxy resin and may be used as fillers. There are a number of requirements which should be met.
  • the solid particles must be compatible with the components of epoxy varnishes formulated for use in glass reinforced laminates. They should be resistant to aggressive solvents such as DMF and acetone. They should be of a size which permits good dispersion through the mixture. They should not be too large relative to the distance between the circuit lines since they will affect the electrical properties. They should not agglomerate. They should not have significant effect on high temperature tests which laminates must meet, such as solder float. Their density should be similar to that of epoxy resin so that they neither tend to settle or float on the surface. These properties have been found to be satisfied by the polymeric particles described below.
  • the benefits of the present invention may be achieved with the use of particles which have a uniform composition throughout, the preferred particles are those which are commonly called “core-shell” particles.
  • U.S. Pat. No. 3,426,101 describes the process in detail.
  • a recent patent disclosing the use of such particles in amo ⁇ hous aromatic polyesters to improve impact strength is U. S. Pat. No. 5,409,967.
  • the use of such particles to provide toughening of epoxy resins is also known, as is discussed in the article by B.J. Cardwell and A.F. Yee in Polvmer. 1993, Volume 34, Number 8, p. 1695-1701.
  • a rubber-modified phenolic resin is made by heating the resin to soften and to disperse rubber particles in the resin.
  • the phenolic resin is later combined with an epoxy resin and an inorganic filler for use as an encapsulant, where it is said to have good impact resistance and thermal shock resistance.
  • Core-shell particles are made by suspension polymerization of a rubbery polymer in which very small seed particles (the core) are produced. Then, the shell is formed over the rubbery core by introducing a monomer which polymerizes to form a hard coating on the surface of the core. This is done under conditions which form little or no. separate, particles o the shell polymer, but which cause the second monomeE to be formed , over the core instead.
  • the particles generally will have an average diameter of about 0.05 to 30 ⁇ m, preferably about 0.05 to 5 ⁇ m.
  • I 5 polymers is not considered to be critical, a preferred particle has a core of butadiene crosslinked with a second monomer and covered with a shell comprising a methacrylate polymer.
  • the butadiene polymer has good chemical resistance and high temperature; however, it is rubbery and the harder shell
  • polymer is needed to minimize agglomeration and improve mixing with the epoxy resin.
  • the shall polymer is more likely to be attacked by the solvents, although this may be advantageous in the present application.
  • Inorganic particles such as talc, wollastonite (Ca silicate),
  • Inorganic fillers are disclosed in U.S. Pat. No. 5,264,065 to be useful in controlling the coefficient of thermal expansion in the Z-axis of laminates, generally using 30 to 100 parts of filler per hundred of resin. Such fillers have been used in laminates for other and related purposes according to the Japanese patent applications discussed in the '065 U.S. patent.
  • CEM-3 laminates are made by impregnating a non-woven glass fiber mat with an epoxy resin formulation and then B-staging the impregnated mat.
  • B-staging means that the epoxy resin is partially cured so that it is not tacky and can be handled and stored for some time before being used to make a finished laminate.
  • prepregs Such materials are often called "prepregs”.
  • covering layers of prepregs made by impregnating woven glass cloth with an epoxy resin formulation are placed on either side ofthe B-staged mat and the composite is cured to produce a CEM-3 substrate.
  • C-staged When assembled with copper foils and other layers of prepreg or fully cured composites they can be cured under heat and pressure to complete the curing process (C-staged).
  • the layers may be reversed, that is, a woven glass cloth may be used in the center with covering layers of non-woven glass 0 fiber mats.
  • Such structures have been found to resist wa ⁇ ing and twisting better than conventional CEM-3
  • the dielectric constant and dissipation factor of epoxy resin materials are not as low as might be desired.
  • the inventors have - > sought and have found a method for improving such electrical properties, while at the same time not degrading the usual properties of CEM-3 composites.
  • the objective has been to increase the ability of the epoxy resin to prevent the passage of electricity as defined by the dielectric constant and the dissipation 0 factor, which have been discussed above. Clearly, this will be a desirable characteristic when higher electrical voltages are in use or when the circuit pattem is very dense so that there is little space between the current carrying copper lines.
  • the amount used should be Q between about 3 and 20 wt.%, based on the resin content.
  • the particle size is an important factor in obtaining the desired results.
  • the average diameter should be between about 0.05 and 30 ⁇ m, preferably about 0.05 and 5 ⁇ m. Larger particles will be difficult to distribute uniformly throughout the epoxy resin and would be expected to weaken the structure if too large.
  • the minimum size ofthe particles is not known, but is presumed to be determined by the method used to make the particles.
  • Example 1 An epoxy varnish containing 20 parts by weight of core-shell particles per hundred weight of epoxy resin (phr) was prepared by dissolving 26.7 grams of dicyandiamide in 395 grams of dimethyl formamide and mixing the resulting solution into 1236 grams of DER 71881 A80 epoxy resin (Dow Chemical). The following were then added to the epoxy resin mixture: 270 grams of acetone, 386 grams of ASP400 (3-5 ⁇ m aluminum silicate powder, Engelhard Co ⁇ .), 288 grams of ATH C330 (3 ⁇ m aluminum trihydrate powder, Alcoa), 42 grams of antimony trioxide, and 198 grams of Paraloid EXL2691 (core-shell particles, Rohm and Haas, 0.1 ⁇ m).
  • a copper clad laminate was made for testing by stacking 4 plies of B-staged mat 13"xl3" (330 x 330 mm), placing a 1 oz/ft 2 (305 grams/m 2 ) copper foil on one side and a 1 mil (25 ⁇ m) thick release film on the other.
  • the stacked layers were placed between two stainless steel caul plates and three layers of Kraft paper were placed on each side of the stack before being pressed at 300°F (149°C) for 20 minutes, and finally at 340°F (171°C) for 80 minutes, using a pressure of 250 psi (1723 kPa).
  • the cured stack was cooled to room temperature while remaining under pressure and then cut to 12" x 12" (304 x 304 mm).
  • the resulting laminate was then tested using standard tests for such laminates, with the results being reported in the table below.
  • Example 2 The procedure of Example 1 was repeated except that the proportion of Paraloid 2691 was reduced to one-half, 10 parts per hundred of epoxy resin (phr) or 8.35 wt.% of the B-staged mat. The cured laminate was measured as before and the results are shown in the table below.
  • Example 3 The procedure of Example 1 and 2 was repeated except that the amount of Paraloid 2691 was cut in half again, that is to 5 pph resin or 4.18 wt % based on the B-staged mat. The properties of the cured laminate were measured and the results reported below.
  • Example 4 (comparative ⁇ The experiments of the above examples were repeated except that no Paraloid 2691 was used, but instead 7.5 pph of Hycar elastomer (B.F. Goodrich) was included in the resin formulation. The finished laminate was measured as before and the results are shown below.
  • Example 5 (comparative) Another laminate was prepared as in the above examples except that no Paraloid was included and no elastomer was added as in Example 4. Properties of this base laminate are reported in the table below.
  • Example 6 The procedure of Example 6 was repeated using 15 phr of Paraloid EXL2691 and talc (Nytal 400, 3-5 ⁇ m, R.T. Vanderbilt) was substituted for the ASP400. The laminate was tested as before, with the results shown in the table below.
  • compositions T and TLP which contain talc and no calcium silicate have undesirably low values in the solder float test. Also, reducing the amount of Paraloid (T vs. TLP) sha ⁇ ly reduces the CTI to an unacceptable value.
  • Example 9 Three similar formulations were prepared employing varying amounts of inorganic fillers, each including the polymeric filler Paraloid EXL
  • compositions were: Component A B TC
  • composition TC has superior performance in the Comparative Tracking Index test and exhibits a good resistance in the solder float test.
  • This composition includes talc and calcium silicate, but omits aluminum trihydrate, which is considered to be the reason for undesirably low results in the solder float test.

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  • Engineering & Computer Science (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Laminated Bodies (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

Les circuits imprimés sont constitués de plaquettes qui, comme les plaquettes CEM-3, comportent des substrats isolants renfermant des particules polymères, notamment des particules à noyau et enveloppe d'un calibre moyen situé entre environ 0,05 et 30 microns, ce qui atténue la constante diélectrique et le facteur de dissipation de ces plaquettes. L'indice comparatif d'alignement se trouve sensiblement amélioré.
PCT/US1996/016400 1995-10-10 1996-10-10 Plaquettes pour circuit imprime a caracteristiques dielectriques ameliorees Ceased WO1997014280A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU72646/96A AU7264696A (en) 1995-10-10 1996-10-10 Laminates having improved dielectric properties

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US54441895A 1995-10-10 1995-10-10
US08/544,418 1995-10-10

Publications (1)

Publication Number Publication Date
WO1997014280A1 true WO1997014280A1 (fr) 1997-04-17

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PCT/US1996/016400 Ceased WO1997014280A1 (fr) 1995-10-10 1996-10-10 Plaquettes pour circuit imprime a caracteristiques dielectriques ameliorees

Country Status (3)

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AU (1) AU7264696A (fr)
TW (1) TW370490B (fr)
WO (1) WO1997014280A1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1051061A1 (fr) * 1999-05-03 2000-11-08 JSR Corporation Composition à constante diélectrique faible, matériau isolant, matériau d'étanchéité, et plaque de circuit
US6288169B1 (en) * 1998-04-23 2001-09-11 Nitto Denko Corporation Butadiene rubber particles with secondary particle sizes for epoxy resin encapsulant
US6949289B1 (en) 1998-03-03 2005-09-27 Ppg Industries Ohio, Inc. Impregnated glass fiber strands and products including the same
US7354641B2 (en) 2004-10-12 2008-04-08 Ppg Industries Ohio, Inc. Resin compatible yarn binder and uses thereof

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6753483B2 (en) 2000-06-14 2004-06-22 Matsushita Electric Industrial Co., Ltd. Printed circuit board and method of manufacturing the same

Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS63154748A (ja) * 1986-12-18 1988-06-28 Sumitomo Bakelite Co Ltd 熱硬化性樹脂積層板
JPS63159441A (ja) * 1986-12-23 1988-07-02 Sumitomo Bakelite Co Ltd 熱硬化性樹脂積層板
JPS63268637A (ja) * 1987-04-28 1988-11-07 Asahi Glass Co Ltd 金属箔張積層板
JPH0314282A (ja) * 1989-06-13 1991-01-22 Mitsubishi Electric Corp 低誘電率プリント基板
US5216077A (en) * 1988-01-06 1993-06-01 Kabushiki Kaisha Toshiba Rubber-modified phenolic resin composition and method of manufacturing the same
JPH05162241A (ja) * 1991-12-16 1993-06-29 Matsushita Electric Works Ltd 積層板
JPH05162240A (ja) * 1991-12-16 1993-06-29 Matsushita Electric Works Ltd 積層板
JPH06338667A (ja) * 1993-05-28 1994-12-06 Sumitomo Bakelite Co Ltd 印刷回路用片面銅張積層板

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS63154748A (ja) * 1986-12-18 1988-06-28 Sumitomo Bakelite Co Ltd 熱硬化性樹脂積層板
JPS63159441A (ja) * 1986-12-23 1988-07-02 Sumitomo Bakelite Co Ltd 熱硬化性樹脂積層板
JPS63268637A (ja) * 1987-04-28 1988-11-07 Asahi Glass Co Ltd 金属箔張積層板
US5216077A (en) * 1988-01-06 1993-06-01 Kabushiki Kaisha Toshiba Rubber-modified phenolic resin composition and method of manufacturing the same
JPH0314282A (ja) * 1989-06-13 1991-01-22 Mitsubishi Electric Corp 低誘電率プリント基板
JPH05162241A (ja) * 1991-12-16 1993-06-29 Matsushita Electric Works Ltd 積層板
JPH05162240A (ja) * 1991-12-16 1993-06-29 Matsushita Electric Works Ltd 積層板
JPH06338667A (ja) * 1993-05-28 1994-12-06 Sumitomo Bakelite Co Ltd 印刷回路用片面銅張積層板

Non-Patent Citations (8)

* Cited by examiner, † Cited by third party
Title
B.J. CARDWELL ET AL.: "Rate and temperature effects on the fracture toughness of a rubber-modified epoxy", POLYMER, vol. 34, no. 7, March 1993 (1993-03-01), pages 1695 - 1701, XP000609999 *
DATABASE WPI Week 8831, Derwent World Patents Index; AN 88-217586, XP002022155 *
DATABASE WPI Week 8832, Derwent World Patents Index; AN 88-224301, XP002022154 *
DATABASE WPI Week 8850, Derwent World Patents Index; AN 88-357643, XP002022156 *
DATABASE WPI Week 9330, Derwent World Patents Index; AN 93-239607, XP002022158 *
DATABASE WPI Week 9330, Derwent World Patents Index; AN 93-239608, XP002022157 *
PATENT ABSTRACTS OF JAPAN vol. 15, no. 130 (E - 1051) 29 March 1991 (1991-03-29) *
PATENT ABSTRACTS OF JAPAN vol. 95, no. 3 28 April 1995 (1995-04-28) *

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6949289B1 (en) 1998-03-03 2005-09-27 Ppg Industries Ohio, Inc. Impregnated glass fiber strands and products including the same
US6288169B1 (en) * 1998-04-23 2001-09-11 Nitto Denko Corporation Butadiene rubber particles with secondary particle sizes for epoxy resin encapsulant
US6596813B2 (en) 1998-04-23 2003-07-22 Nitto Denko Corporation Composition of epoxy resin, phenolic resin, butadiene particles and amino silicone oil
US6962957B2 (en) 1998-04-23 2005-11-08 Nitto Denko Corporation Epoxy resin composition for semiconductor encapsulation, process for producing the same, and semiconductor device
EP1051061A1 (fr) * 1999-05-03 2000-11-08 JSR Corporation Composition à constante diélectrique faible, matériau isolant, matériau d'étanchéité, et plaque de circuit
US6146749A (en) * 1999-05-03 2000-11-14 Jsr Corporation Low dielectric composition, insulating material, sealing material, and circuit board
US7354641B2 (en) 2004-10-12 2008-04-08 Ppg Industries Ohio, Inc. Resin compatible yarn binder and uses thereof

Also Published As

Publication number Publication date
AU7264696A (en) 1997-04-30
TW370490B (en) 1999-09-21

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