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

Haihong Bao, Yuan Qiu, Xianyun Peng, Jia-ao Wang, Yuying Mi, Shunzheng Zhao, Xijun Liu (), Yifan Liu, Rui Cao (), Longchao Zhuo, Junqiang Ren, Jiaqiang Sun, Jun Luo and Xuping Sun ()
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Haihong Bao: Tianjin University of Technology
Yuan Qiu: Tianjin University of Technology
Xianyun Peng: Tianjin University of Technology
Jia-ao Wang: University of Jinan
Yuying Mi: Tianjin University of Technology
Shunzheng Zhao: University of Science and Technology Beijing
Xijun Liu: Tianjin University of Technology
Yifan Liu: Shenzhen University
Rui Cao: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Longchao Zhuo: Xi’an University of Technology
Junqiang Ren: Lanzhou University of Technology
Jiaqiang Sun: Institute of Coal Chemistry, Chinese Academy of Sciences
Jun Luo: Tianjin University of Technology
Xuping Sun: University of Electronic Science and Technology of China

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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 Ti3C2Tx 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–O3 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.

Date: 2021
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DOI: 10.1038/s41467-020-20336-4

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