Issue 14, 2022

Regulating the interfacial water structure by tensile strain to boost electrochemical semi-hydrogenation of alkynes

Abstract

Electrochemical semi-hydrogenation (ECSH) of alkynes to produce alkenes is an ideal alternative to traditional thermal semi-hydrogenation (TSH) and yet is limited by low conversion yield and product selectivity. Here, we report a new strategy to tune the activity and selectivity of ECSH by regulating the interfacial water structure. The obtained PdCu icosahedrons deliver a greatly enhanced conversion rate and 98.5% alkene selectivity at 96.5% conversion, as well as sustaining about 100 h continuous test. Tensile strain originating from an icosahedral twinned structure is proved to facilitate the formation of an interfacial water structure, especially K+ ion hydrated water (K·H2O) and 2-coordinated hydrogen-bonded water (2-HB·H2O). We also decode the mysterious role of an interfacial water structure in ECSH performance, in which K·H2O speeds up water splitting to produce Hads which in turn accelerates ECSH conversion, and 2-HB·H2O improves alkene selectivity. The findings provide insights into the tuning of the interfacial water structure in electrocatalyst design in proton-coupled hydrogenation from the viewpoint of lattice strain.

Graphical abstract: Regulating the interfacial water structure by tensile strain to boost electrochemical semi-hydrogenation of alkynes

Supplementary files

Article information

Article type
Research Article
Submitted
10 四月 2022
Accepted
30 五月 2022
First published
31 五月 2022

Inorg. Chem. Front., 2022,9, 3444-3452

Regulating the interfacial water structure by tensile strain to boost electrochemical semi-hydrogenation of alkynes

X. Xu, J. Ma, F. Wu, K. Zhu, H. Zhou, Y. Zhang, X. Li, Y. Zhou, G. Jia, D. Liu, P. Gao and W. Ye, Inorg. Chem. Front., 2022, 9, 3444 DOI: 10.1039/D2QI00767C

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