Partially charged single-atom Ru supported on ZrO2 nanocrystals for highly efficient ethylene hydrosilylation with triethoxysilane

Homogeneous noble metal catalysts used in alkene hydrosilylation reactions to manufacture organosilicon compounds commercially often suffer from difficulties in catalyst recovering and recycling, undesired disproportionation reactions, and energy-intensive purification of products. Herein, we report a heterogeneous 0.5Ru(delta+)/ZrO2 catalyst with partially charged single-atom Ru (0.5 wt.% Ru) supported on commercial ZrO2 nanocrystals synthesized by the simple impregnation method followed by H-2 reduction. When used in the ethylene hydrosilylation with triethoxysilane to produce the desired ethyltriethoxysilane, 0.5Ru(delta+)/ZrO2 showed excellent catalytic performance with the maximum Ru atom utilization and good recyclability, even superior to homogeneous catalyst (RuCl3 center dot H2O). Structural characterizations and density functional theory calculations reveal the atomic dispersion of the active Ru species and their unique electronic properties distinct from the homogeneous catalyst. The reaction route over this catalyst is supposed to follow the typical Chalk-Harrod mechanism. This highly efficient and supported single-atom Ru catalyst has the potential to replace the current homogeneous catalyst for a greener hydrosilylation industry.

Automated summary

This study reports a heterogeneous 0.5Ru(delta+)/ZrO2 catalyst with excellent catalytic performance and recyclability for producing ethyltriethoxysilane through ethylene hydrosilylation. Structural characterizations and theoretical calculations reveal the atomic dispersion and unique electronic properties of the active Ru species on the catalyst, which has the potential to replace homogeneous catalysts for a greener hydrosilylation industry.