US 12,104,113 B2
Thermally conductive silicone composition, production method thereof, and semiconductor device
Takahiro Yamaguchi, Annaka (JP)
Assigned to SHIN-ETSU CHEMICAL CO., LTD., Tokyo (JP)
Appl. No. 17/762,844
Filed by SHIN-ETSU CHEMICAL CO., LTD., Tokyo (JP)
PCT Filed Sep. 7, 2020, PCT No. PCT/JP2020/033738
§ 371(c)(1), (2) Date Mar. 23, 2022,
PCT Pub. No. WO2021/059936, PCT Pub. Date Apr. 1, 2021.
Claims priority of application No. 2019-177423 (JP), filed on Sep. 27, 2019.
Prior Publication US 2022/0275265 A1, Sep. 1, 2022
Int. Cl. C09K 5/08 (2006.01); H01L 23/373 (2006.01)
CPC C09K 5/08 (2013.01) [H01L 23/3737 (2013.01)] 12 Claims
 
1. A heat-conductive silicone composition comprising:
(A) 100 parts by weight of an organopolysiloxane of general formula (1) below

OG Complex Work Unit Chemistry
(wherein each R is a substituted or unsubstituted monovalent hydrocarbon group of 1 to 20 carbon atoms, multiple occurrences of R may be the same or may be different, and n is an integer of 10 or more);
(B) from 150 to 600 parts by weight of an organopolysiloxane of general formula (2) below having at least one hydrolyzable silyl group per molecule

OG Complex Work Unit Chemistry
(wherein each R1 is independently a substituted or unsubstituted monovalent hydrocarbon group, X1 and X3 are each independently a group represented by R1 or —R2—SiR3g(OR4)3-g, and X2 is a group represented by —R2—SiR3g(OR4)3-g, there being at least one —R2—SiR3g(OR4)3-g moiety on the molecule; R2 is an oxygen atom or an alkylene group of 1 to 4 carbon atoms, each R3 is independently a substituted or unsubstituted monovalent hydrocarbon group which does not contain an aliphatic unsaturated bond, each R4 is independently an alkyl group of 1 to 4 carbon atoms or an alkoxyalkyl, alkenyl or acyl group of 2 to 4 carbon atoms, and g is an integer from 0 to 2; the subscripts a and b respectively satisfy the conditions 1≤a≤1,000 and 0≤b≤1,000, with the proviso that if X1 and X3 are both R1, b satisfies the condition 1≤b≤1,000; and recurring units may each be randomly bonded);
(C) from 0.1 to 100 parts by weight of a crosslinking agent which is a hydrolyzable organosilane compound having one unsubstituted monovalent hydrocarbon group selected from the group consisting of alkyl groups of 1 to 4 carbon atoms, alkenyl groups of 2 to 4 carbon atoms and aryl groups of 6 to 8 carbon atoms and three hydrolyzable groups per molecule and/or a partial hydrolytic condensation product thereof;
(D) from 1,500 to 6,500 parts by weight of zinc oxide particles which have a mean particle diameter of at least 0.1 μm but not more than 2 μm and contain a proportion of coarse product having a particle diameter of 10 μm or more in laser diffraction particle size distribution that is not more than 1 vol % of component (D) overall; and
(E) from 0.01 to 30 parts by weight of an adhesion promoter exclusive of component (C), wherein the composition has a content of component (D) that is from 45 to 70 vol % of the overall composition and a thermal conductivity at 25° C. as determined by the hot disk method of at least 1.3 W/mK, and is compressible to a thickness of 10 μm or less.