Mediating trade-off between activity and selectivity in alkynes semi-hydrogenation via a hydrophilic polar layer

Jinqi Xiong, Shanjun Mao (), Qian Luo, Honghui Ning, Bing Lu, Yanling Liu and Yong Wang ()
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Jinqi Xiong: Zhejiang University
Shanjun Mao: Zhejiang University
Qian Luo: Zhejiang University
Honghui Ning: Zhejiang University
Bing Lu: Zhejiang University
Yanling Liu: Zhejiang University
Yong Wang: Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract As a crucial industrial process for the production of bulk and fine chemicals, semi-hydrogenation of alkynes faces the trade-off between activity and selectivity due to undesirable over-hydrogenation. By breaking the energy linear scaling relationships, we report an efficient additive-free WO3-based single-atom Pd catalytic system with a vertical size effect of hydrogen spillover. Hydrogen spillover induced hydrophilic polar layer (HPL) with limited thickness on WO3-based support exhibits unconventional size effect to Pd site, in which over-hydrogenation is greatly suppressed on Pd1 site due to the polar repulsive interaction between HPL and nonpolar C=C bonds, whereas this is invalid for Pd nanoparticles with higher altitudes. By further enhancing the HPL through Mo doping, activated Pd1/MoWO3 achieves recorded performance of 98.4% selectivity and 10200 h−1 activity for semi-hydrogenation of 2-methyl-3-butyn-2-ol, 26-fold increase in activity of Lindlar catalyst. This observed vertical size effect of hydrogen spillover offers broad potential in catalytic performance regulation.

Date: 2024
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DOI: 10.1038/s41467-024-45104-6

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