Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products.

Bao, Haihong; Qiu, Yuan; Peng, Xianyun; Wang, Jia-Ao; Mi, Yuying; Zhao, Shunzheng; Liu, Xijun; Liu, Yifan et al. · Nat Commun · 2021

basic_science · Level V

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Abstract

Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at -0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu-O<sub>3</sub> sites favor the C-C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.