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

TY - JOUR

T1 - Partially charged single-atom Ru supported on ZrO2 nanocrystals for highly efficient ethylene hydrosilylation with triethoxysilane

AU - Li, Mingyan

AU - Zhao, Shu

AU - Li, Jing

AU - Chen, Xiao

AU - Ji, Yongjun

AU - Yu, Haijun

AU - Bai, Dingrong

AU - Xu, Guangwen

AU - Zhong, Ziyi

AU - Su, Fabing

PY - 2022

Y1 - 2022

N2 - 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 0.5Ruδ+/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 H2 reduction. When used in the ethylene hydrosilylation with triethoxysilane to produce the desired ethyltriethoxysilane, 0.5Ruδ+/ZrO2 showed excellent catalytic performance with the maximum Ru atom utilization and good recyclability, even superior to homogeneous catalyst (RuCl3·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.

AB - 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 0.5Ruδ+/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 H2 reduction. When used in the ethylene hydrosilylation with triethoxysilane to produce the desired ethyltriethoxysilane, 0.5Ruδ+/ZrO2 showed excellent catalytic performance with the maximum Ru atom utilization and good recyclability, even superior to homogeneous catalyst (RuCl3·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.

U2 - 10.1007/s12274-022-4227-4

DO - 10.1007/s12274-022-4227-4

M3 - 文章

SN - 1998-0124

JO - Nano Research

JF - Nano Research

ER -