Effect of segment structure of monotrimethoxysilylethyl-terminated asymmetric polysiloxanes on the thermal management performance of AlN-filled silicone pastes

Abstract

Three kinds of α-triethylsiloxyl-ω-trimethoxysilyethyl-terminated oligomers (TES-PDMS-TMOS, TES-PTFPMS-TMOS, and TES-PDES-TMOS) were synthesized through an anion catalyzed non-equilibrium ring-opening polymerization reaction of cyclotrisiloxanes and subsequent hydrosilylation reaction with vinyltrimethoxysilane. As the in situ surface modification agent for mixed-size AlN inorganic fillers (1, 20 and 50 μm blended in a mass ratio of 3:5:9), these oligomers have been mixed with Vi-PDMS in a mass ratio of 1:2. Relative to that of silicone pastes using Vi-PDMS as the polymer matrix, the thermal conductivity of silicone pastes made from AlN particles treated with these oligomers is enhanced, while their thermal resistances decreased. With the change of the repeating unit structure in the oligomers, the silicone pastes prepared from these oligomer-treated AlN fillers differ significantly in filler content, thermal conductivity, and thermal resistance. When TES-PTFPMS-TMOS is used and filled with 800 parts (70.3 vol%) of hybrid AlN powders, a silicone paste with a thermal conductivity of 4.56 W/(m. K) could be achieved, which was 37.8% higher than that silicone paste using pure Vi-PDMS as the matrix. When TES-PDES-TMOS is used and filled with 900 parts (72.7 vol%) of hybrid AlN powders, the thermal conductivity of the silicone paste reaches 4.13 W/(m. K). Despite its thermal conductivity being only 3.5% higher relative to the silicone paste using only Vi-PDMS as the polymer matrix, its thermal resistance decreased by 20.3%. When TES-PDMS-TMOS is used and filled with 1200 parts (78.0 vol%) of hybrid AlN powders, the thermal conductivity of the silicone paste could reach up to 4.59 W/(m. K), together with a thermal resistance 29.6% lower than that of silicone paste where 1000 parts (74.7 vol%) of hybrid AlN particles filled in the Vi-PDMS. The heat dissipation of the 30 W high-brightness LED chip also illustrated the excellent thermal conductivities of these silicone pastes. The effect of another terminal group on the monotrimethoxysilylethyl-terminated asymmetric polysiloxanes on the thermal resistance of thermal interface materials was also discussed in detail.