Method for forming thermally conductive thermal radical cure silicone compositions

Patent metadata

Field	Value
Publication number	US-10370574-B2
Application number	US-201414766774-A
Country	US
Kind code	B2
Filing date	Feb 10, 2014
Priority date	Feb 11, 2013
Publication date	Aug 6, 2019
Grant date	Aug 6, 2019

Abstract

A method for forming a thermally conductive thermal radical cure silicone composition comprising (I) a clustered functional polyorganopolysiloxane; optionally (II) a silicone reactive diluent, (III) a filler comprising a thermally conductive filler, (III′) a filler treating agent, and (IV) a radical initiator is provided. In this method, the clustered functional polyorganosiloxane (I) and the optional silicone reactive diluent (II) are premade prior to their addition to respective components (III), (III′) and (IV).

First claim

The invention claimed is:

1. A method for forming a thermally conductive thermal radical cure silicone composition comprising (I) a clustered functional polyorganopolysiloxane; (II) a silicone reactive diluent; (III) a filler comprising a thermally conductive filler, (III′) a filler treating agent, and (IV) a radical initiator, the method comprising:
(A) providing a clustered functional polyorganosiloxane (I) that comprises a reaction product of a reaction of:
a) a polyorganosiloxane having an average, per molecule, of at least 2 aliphatically unsaturated organic groups,
b) a polyorganohydrogensiloxane having an average, per molecule, of 4 to 15 silicon atoms and at least 4 silicon bonded hydrogen atoms per aliphatically unsaturated organic group in component a),
c) a reactive species having, per molecule at least one aliphatically unsaturated organic group and one or more curable groups selected from acrylate groups and methacrylate groups, and
in the presence of d) a hydrosilylation catalyst and e) an isomer reducing agent, wherein the isomer reducing agent is present in an amount based on the total weight of the clustered functional polyorganosiloxane (I) to produce at least a 10% reduction in beta-addition of SiH groups to the polyorganosiloxane to the aliphatically unsaturated group of the reactive species as compared to a clustered functional polyorganosiloxane formed in the absence of the isomer reducing agent;
(B) forming a first mixture by mixing the filler (III) comprising the thermally conductive filler, the filler treating agent (III′), and at least one of the silicone reactive diluent (II) and the clustered functional polyorganosiloxane (I);
(C) heating the first mixture to a temperature from 50° C. to 110° C. to treat the thermally conductive filler (III) with the filler treating agent (III′)
(D) after heating in step (C), introducing the silicone reactive diluent (II), the clustered functional polyorganosiloxane (I), or neither to the first mixture as needed to obtain a final mixture that comprises both the silicone reactive diluent (II) and the clustered functional polyorganosiloxane (I); and then
(E) cooling the final mixture to 30° C. or less and then blending a radical initiator (IV) with the final mixture to form a thermally conductive thermal radical cure silicone composition.

2. The method according to claim 1 further comprising:
(F) blending at least one additional component with the final mixture prior to Step (E), the at least one additional component selected from the group consisting of (III) an additional amount of filler comprising the thermally conductive filler, (III′) an additional amount of filler treating agent, (V) a moisture cure initiator, (VI) a crosslinker, (VII) a moisture cure polymer, (VIII) a solvent, (IX) an adhesion promoter, (X) a colorant, (XI) a reactive diluent, (XII) a corrosion inhibitor, (XIII) a polymerization inhibitor, (XIV) an acid acceptor, and any combination thereof,
wherein, after performing Step (F), the final mixture to be used in Step (E) comprises the at least one additional component.

3. The method as set forth in claim 2 , wherein the (VI) crosslinker and the moisture cure polymer (VII) are both present in the thermally conductive thermal radical cure silicone composition and wherein the amount of the crosslinker (VI) comprises from 0.001 to 50 weight percent of the total weight of moisture cure polymer (VII) and wherein the amount of the moisture cure polymer (VII) comprises from 0.1 to 5 weight percent of the total weight of thermally conductive thermal radical cure silicone composition.

4. The method as set forth in claim 2 , wherein the moisture cure polymer (VII) comprises an organopolysiloxane polymer of the formula: (OR 7 ) 3-z R 6 z Si-Q-(R 25 2 SiO 2/2 ) y -Q-SiR 6 z (OR 7 ) 3-z , wherein each R 25 is independently a monovalent hydrocarbon group having 1 to 6 carbon atoms, each R 6 independently is a monovalent hydrocarbon group having 1 to 6 carbon atoms, each R7 independently is selected from the group consisting of a alkyl group and alkoxyalkyl group, Q is a divalent linking group, the subscript z has a value of 0, 1 or 2, and the subscript y has a value of 60 to 1000.

5. The method according to claim 1 , wherein the silicone reactive diluent (II) comprises a reaction product of a reaction of:
a) a polyorganohydrogensiloxane having an average of 10 to 200 silicon atoms per molecule, and
b) a second reactive species having, per molecule, at least 1 aliphatically unsaturated organic group and 1 or more curable groups,
in the presence of c) a second isomer reducing agent and d) a second hydrosilylation catalyst and e) inhibitor for the second hydrosilylation catalyst.

6. The method according to claim 1 , wherein the silicone reactive diluent (II) comprises a reaction product of a reaction of:
a) a siloxane compound according to the formula:

wherein:
R is a monovalent hydrocarbon having 1 to 6 carbon atoms,
R′ is a divalent hydrocarbon having 3 to 12 carbon atoms,
R″ is H or CH 3 , and
the subscripts m and n independently have a value from 1 to 10, and

b) a second polyorganosiloxane having an average, per molecule, of at least 2 aliphatically unsaturated organic groups,
in the presence of c) a second hydrosilylation catalyst and d) an inhibitor for the second hydrosilylation catalyst.

7. The method according to claim 1 , wherein the silicone reactive diluent (II) comprises from 20 to 90 weight percent of a total combined weight of the clustered functional polyorganosiloxane (I) and the silicone reactive diluent (II) in the thermally conductive thermal radical cure silicone composition.

8. The method according to claim 1 , wherein the thermally conductive filler comprises from 30 to 80 volume percent of the total volume of the thermally conductive thermal radical cure silicone composition.

9. The method according to claim 1 , wherein the clustered functional polyorganosiloxane (I) comprises from 20 to 99.9 weight percent of a total combined weight of the clustered functional polyorganosiloxane (I) and the silicone reactive diluent (II) in the thermally conductive thermal radical cure silicone composition.

Assignees

• Dow Silicones Corp

Inventors

• Tan Arianne
• Tang Yin
• Tonge James

Classifications

• C09J183/06

  containing silicon bound to oxygen-containing groups (C09J183/12 takes precedence) · CPC title

• C09K5/14 Primary

  Solid materials, e.g. powdery or granular · CPC title

• C09J183/14

  in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms (C09J183/10 takes precedence) · CPC title

• C09D183/04

  Polysiloxanes · CPC title

• C08G77/12

  containing silicon bound to hydrogen · CPC title