# US 11,077,647 B2 · Thermally conductive silicone rubber composite sheet

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- Number: US 11,077,647 B2
- Document ID: US11077647B2
- Status: Granted
- Kind: B2
- Application number: 16/313,795
- Filed: 2017-07-12
- Published: 2020-04-23
- Granted: 2021-08-03
- Earliest claimed: 2016-08-05
- Assignees: Shin-Etsu Chemical Co., Ltd.
- Applicants: Shin-Etsu Chemical Co., Ltd.
- Inventors: Akihiro Endo; Yuki Tanaka
- Web page: https://patentgrep.com/patent/US11077647B2

## CPC

- B32B 27/281: {comprising polyimides}
- C08J 5/18: Manufacture of films or sheets
- C08J 7/042: {with two or more layers, where at least one layer of a composition contains a polymer binder}
- C08J 7/0427: {with only one layer of a composition containing a polymer binder (with more layers C08J7/042)}
- C08J 7/043: Improving the adhesiveness of the coatings per se, e.g. forming primers (adhesives in the form of films or foils characterised by the primer layers between the polymer carriers and the adhesives C09J7/50)
- C08J 7/044: Forming conductive coatings; Forming coatings having anti-static properties
- C08K 3/22: of metals
- C09D 5/00: Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced {(electrically insulating plastics, resins or waxes H01B3/30)}; Filling pastes
- C09D 7/61: inorganic
- C09D 183/04: Polysiloxanes
- C09K 5/14: Solid materials, e.g. powdery or granular
- H10W 40/10: Arrangements for heating
- H10W 40/25: characterised by their materials
- H10W 40/251: {Organics}
- H10W 40/255: {having a laminate or multilayered structure, e.g. direct bond copper [DBC] ceramic substrates}
- B32B 2255/10: on synthetic resin layer or on natural or synthetic rubber layer
- B32B 2255/26: Polymeric coating
- B32B 2264/102: Oxide or hydroxide
- B32B 2307/206: Insulating
- B32B 2307/302: Conductive
- B32B 2307/546: Flexural strength; Flexion stiffness
- B32B 2457/00: Electrical equipment
- C08J 2379/08: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- C08J 2483/04: Polysiloxanes
- C08J 2483/07: containing silicon bound to unsaturated aliphatic groups
- C08K 2003/2227: {of aluminium}
- C08K 2201/001: Conductive additives
- B32B: LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- C08J: WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H (working, e.g. shaping, of plastics B29)
- C08K: Use of inorganic or non-macromolecular organic substances as compounding ingredients (paints, inks, varnishes, dyes, polishes, adhesives C09)
- C09D: COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR (cosmetics A61K; processes for applying liquids or other fluent materials to surfaces, in general, B05D; staining wood B27K5/02; glazes or vitreous enamels C03C; natural resins, French polish, drying-oils, driers, turpentine, per se, C09F; polishing compositions other than French polish, ski waxes C09G; adhesives or use of materials as adhesives C09J; materials for sealing or packing joints or covers C09K3/10; materials for stopping leaks C09K3/12; processes for the electrolytic or electrophoretic production of coatings C25D)
- C09K: MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- H10W: GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10

## Abstract

Provided is an inexpensive thermally conductive silicone rubber composite sheet. The thermally conductive silicone rubber composite sheet of the invention includes a laminated structure body comprised of an intermediate layer and an outer layer laminated on both surfaces of the intermediate layer, in which (A) the intermediate layer is an electrical insulating synthetic resin film layer having a thermal conductivity of not lower than 0.20 W/m·K and a tensile elastic modulus of not lower than 5 GPa, and (B) the outer layer is a silicone rubber layer of a cured product of a composition containing: (a) an organopolysiloxane; (b) a curing agent; (c) a thermally conductive filler; and (d) a silicon compound-based adhesion imparting agent having at least one kind of group selected from the group consisting of an epoxy group, an alkoxy group, a methyl group, a vinyl group and a Si—H group.

## Claims

### Claim 1

A thermally conductive silicone rubber composite sheet including a laminated structure body comprised of an intermediate layer and an outer layer laminated on both surfaces of the intermediate layer, wherein
(A) the intermediate layer is an electrically insulating synthetic resin film layer having a thermal conductivity of not lower than 0.20 W/m·K, a tensile elastic modulus of not lower than 5 GPa, and a thickness of 50 to 100 μm, and
(B) the outer layer is a silicone rubber layer of a cured product of a composition containing: (a) an organopolysiloxane; (b) a curing agent; (c) a thermally conductive filler; and (d) a silicon compound-based adhesion imparting agent having at least one kind of group selected from the group consisting of an epoxy group, an alkoxy group, a methyl group, a vinyl group and a Si—H group.

### Claim 2 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein the thermally conductive silicone rubber composite sheet has a total thickness of not larger than 300 μm.

### Claim 3 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein the intermediate layer has a tensile strength of not lower than 200 MPa.

### Claim 4 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein a synthetic resin used in the synthetic resin film layer is an aromatic polyimide, a polyamide, a polyamideimide, a polyester or a fluorine-based polymer; or a combination of two or more of them.

### Claim 5 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein a synthetic resin used in the synthetic resin film layer is a polyimide as a polycondensate of biphenyltetracarboxylic acid dianhydride and diamine.

### Claim 6 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein a powder as the thermally conductive filler is a zinc oxide powder, an aluminum oxide powder, a magnesium oxide powder, an aluminum hydroxide powder, a boron nitride powder, an aluminum nitride powder, a silicon oxide powder, a silicon carbide powder or a diamond powder; or a combination of two or more of them.

### Claim 7 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein the curing agent as the component (b) is an addition reaction-type curing agent utilizing hydrosilylation reaction, and the silicon compound-based adhesion imparting agent as the component (d) has any one or both of a vinyl group and a Si—H group; and any one or both of an epoxy group and an alkoxy group.

### Claim 8 (depends on 1)

The thermally conductive silicone rubber composite sheet according to claim 1, wherein the curing agent as the component (b) is an organic peroxide, and the silicon compound-based adhesion imparting agent as the component (d) has any one or both of a methyl group and a vinyl group; and any one or both of an epoxy group and an alkoxy group.

### Claim 9 (depends on 2)

The thermally conductive silicone rubber composite sheet according to claim 2, wherein the intermediate layer has a tensile strength of not lower than 200 MPa.

### Claim 10 (depends on 2)

The thermally conductive silicone rubber composite sheet according to claim 2, wherein a synthetic resin used in the synthetic resin film layer is an aromatic polyimide, a polyamide, a polyamideimide, a polyester or a fluorine-based polymer; or a combination of two or more of them.

### Claim 11 (depends on 3)

The thermally conductive silicone rubber composite sheet according to claim 3, wherein a synthetic resin used in the synthetic resin film layer is an aromatic polyimide, a polyamide, a polyamideimide, a polyester or a fluorine-based polymer; or a combination of two or more of them.

### Claim 12 (depends on 9)

The thermally conductive silicone rubber composite sheet according to claim 9, wherein a synthetic resin used in the synthetic resin film layer is an aromatic polyimide, a polyamide, a polyamideimide, a polyester or a fluorine-based polymer; or a combination of two or more of them.

### Claim 13 (depends on 2)

The thermally conductive silicone rubber composite sheet according to claim 2, wherein a synthetic resin used in the synthetic resin film layer is a polyimide as a polycondensate of biphenyltetracarboxylic acid dianhydride and diamine.

### Claim 14 (depends on 3)

The thermally conductive silicone rubber composite sheet according to claim 3, wherein a synthetic resin used in the synthetic resin film layer is a polyimide as a polycondensate of biphenyltetracarboxylic acid dianhydride and diamine.

### Claim 15 (depends on 9)

The thermally conductive silicone rubber composite sheet according to claim 9, wherein a synthetic resin used in the synthetic resin film layer is a polyimide as a polycondensate of biphenyltetracarboxylic acid dianhydride and diamine.

### Claim 16 (depends on 2)

The thermally conductive silicone rubber composite sheet according to claim 2, wherein a powder as the thermally conductive filler is a zinc oxide powder, an aluminum oxide powder, a magnesium oxide powder, an aluminum hydroxide powder, a boron nitride powder, an aluminum nitride powder, a silicon oxide powder, a silicon carbide powder or a diamond powder; or a combination of two or more of them.

### Claim 17 (depends on 3)

The thermally conductive silicone rubber composite sheet according to claim 3, wherein a powder as the thermally conductive filler is a zinc oxide powder, an aluminum oxide powder, a magnesium oxide powder, an aluminum hydroxide powder, a boron nitride powder, an aluminum nitride powder, a silicon oxide powder, a silicon carbide powder or a diamond powder; or a combination of two or more of them.

### Claim 18 (depends on 4)

The thermally conductive silicone rubber composite sheet according to claim 4, wherein a powder as the thermally conductive filler is a zinc oxide powder, an aluminum oxide powder, a magnesium oxide powder, an aluminum hydroxide powder, a boron nitride powder, an aluminum nitride powder, a silicon oxide powder, a silicon carbide powder or a diamond powder; or a combination of two or more of them.

### Claim 19 (depends on 5)

The thermally conductive silicone rubber composite sheet according to claim 5, wherein a powder as the thermally conductive filler is a zinc oxide powder, an aluminum oxide powder, a magnesium oxide powder, an aluminum hydroxide powder, a boron nitride powder, an aluminum nitride powder, a silicon oxide powder, a silicon carbide powder or a diamond powder; or a combination of two or more of them.