Alloying and confinement effects on hierarchically nanoporous CuAu for efficient electrocatalytic semi-hydrogenation of terminal alkynes

Linghu Meng, Cheng-Wei Kao, Zhen Wang, Jun Ma, Peifeng Huang, Nan Zhao, Xin Zheng, Ming Peng, Ying-Rui Lu and Yongwen Tan ()
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Linghu Meng: Hunan University
Cheng-Wei Kao: National Synchrotron Radiation Research Center
Zhen Wang: Hunan University
Jun Ma: Hunan University
Peifeng Huang: Hunan University
Nan Zhao: North China Electric Power
Xin Zheng: North China Electric Power
Ming Peng: Hunan University
Ying-Rui Lu: National Synchrotron Radiation Research Center
Yongwen Tan: Hunan University

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

Abstract: Abstract Electrocatalytic alkynes semi-hydrogenation to produce alkenes with high yield and Faradaic efficiency remains technically challenging because of kinetically favorable hydrogen evolution reaction and over-hydrogenation. Here, we propose a hierarchically nanoporous Cu50Au50 alloy to improve electrocatalytic performance toward semi-hydrogenation of alkynes. Using Operando X-ray absorption spectroscopy and density functional theory calculations, we find that Au modulate the electronic structure of Cu, which could intrinsically inhibit the combination of H* to form H2 and weaken alkene adsorption, thus promoting alkyne semi-hydrogenation and hampering alkene over-hydrogenation. Finite element method simulations and experimental results unveil that hierarchically nanoporous catalysts induce a local microenvironment with abundant K+ cations by enhancing the electric field within the nanopore, accelerating water electrolysis to form more H*, thereby promoting the conversion of alkynes. As a result, the nanoporous Cu50Au50 electrocatalyst achieves highly efficient electrocatalytic semi-hydrogenation of alkynes with 94% conversion, 100% selectivity, and a 92% Faradaic efficiency over wide potential window. This work provides a general guidance of the rational design for high-performance electrocatalytic transfer semi-hydrogenation catalysts.

Date: 2024
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DOI: 10.1038/s41467-024-50499-3

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