Converting copper sulfide to copper with surface sulfur for electrocatalytic alkyne semi-hydrogenation with water

Yongmeng Wu, Cuibo Liu, Changhong Wang, Yifu Yu, Yanmei Shi and Bin Zhang ()
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Yongmeng Wu: Tianjin University
Cuibo Liu: Tianjin University
Changhong Wang: Tianjin University
Yifu Yu: Tianjin University
Yanmei Shi: Tianjin University
Bin Zhang: Tianjin University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Electrocatalytic alkyne semi-hydrogenation to alkenes with water as the hydrogen source using a low-cost noble-metal-free catalyst is highly desirable but challenging because of their over-hydrogenation to undesired alkanes. Here, we propose that an ideal catalyst should have the appropriate binding energy with active atomic hydrogen (H*) from water electrolysis and a weaker adsorption with an alkene, thus promoting alkyne semi-hydrogenation and avoiding over-hydrogenation. So, surface sulfur-doped and -adsorbed low-coordinated copper nanowire sponges are designedly synthesized via in situ electroreduction of copper sulfide and enable electrocatalytic alkyne semi-hydrogenation with over 99% selectivity using water as the hydrogen source, outperforming a copper counterpart without surface sulfur. Sulfur anion-hydrated cation (S2−-K+(H2O)n) networks between the surface adsorbed S2− and K+ in the KOH electrolyte boost the production of active H* from water electrolysis. And the trace doping of sulfur weakens the alkene adsorption, avoiding over-hydrogenation. Our catalyst also shows wide substrate scopes, up to 99% alkenes selectivity, good reducible groups compatibility, and easily synthesized deuterated alkenes, highlighting the promising potential of this method.

Date: 2021
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DOI: 10.1038/s41467-021-24059-y

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