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- Title
Alloying and confinement effects on hierarchically nanoporous CuAu for efficient electrocatalytic semi-hydrogenation of terminal alkynes.
- Authors
Meng, Linghu; Kao, Cheng-Wei; Wang, Zhen; Ma, Jun; Huang, Peifeng; Zhao, Nan; Zheng, Xin; Peng, Ming; Lu, Ying-Rui; Tan, Yongwen
- 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. Electrocatalytic alkyne semi-hydrogenation to alkenes is challenging due to the hydrogen evolution competing reaction and over-hydrogenation. Here, the authors report Cu50Au50 alloy for high selectivity towards styrene production.
- Subjects
CATALYTIC hydrogenation; ALKYNES; HYDROGEN evolution reactions; CATALYST supports; FINITE element method; DENSITY functional theory
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-50499-3