In:
Inorganic Chemistry Frontiers, Royal Society of Chemistry (RSC), Vol. 9, No. 14 ( 2022), p. 3444-3452
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·H 2 O) and 2-coordinated hydrogen-bonded water (2-HB·H 2 O). We also decode the mysterious role of an interfacial water structure in ECSH performance, in which K·H 2 O speeds up water splitting to produce H ads which in turn accelerates ECSH conversion, and 2-HB·H 2 O 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.
Type of Medium:
Online Resource
ISSN:
2052-1553
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
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