Selective CO2 electrolysis to CO using isolated antimony alloyed copper

Jiawei Li, Hongliang Zeng, Xue Dong, Yimin Ding, Sunpei Hu, Runhao Zhang, Yizhou Dai, Peixin Cui, Zhou Xiao, Donghao Zhao, Liujiang Zhou, Tingting Zheng, Jianping Xiao (), Jie Zeng () and Chuan Xia ()
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Jiawei Li: University of Electronic Science and Technology of China
Hongliang Zeng: University of Electronic Science and Technology of China
Xue Dong: University of Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy
Yimin Ding: University of Electronic Science and Technology of China
Sunpei Hu: University of Science and Technology of China
Runhao Zhang: University of Electronic Science and Technology of China
Yizhou Dai: University of Electronic Science and Technology of China
Peixin Cui: Chinese Academy of Sciences
Zhou Xiao: University of Science and Technology of China
Donghao Zhao: University of Science and Technology of China
Liujiang Zhou: University of Electronic Science and Technology of China
Tingting Zheng: University of Electronic Science and Technology of China
Jianping Xiao: University of Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy
Jie Zeng: University of Science and Technology of China
Chuan Xia: University of Electronic Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Renewable electricity-powered CO evolution from CO2 emissions is a promising first step in the sustainable production of commodity chemicals, but performing electrochemical CO2 reduction economically at scale is challenging since only noble metals, for example, gold and silver, have shown high performance for CO2-to-CO. Cu is a potential catalyst to achieve CO2 reduction to CO at the industrial scale, but the C-C coupling process on Cu significantly depletes CO* intermediates, thus limiting the CO evolution rate and producing many hydrocarbon and oxygenate mixtures. Herein, we tune the CO selectivity of Cu by alloying a second metal Sb into Cu, and report an antimony-copper single-atom alloy catalyst (Sb1Cu) of isolated Sb-Cu interfaces that catalyzes the efficient conversion of CO2-to-CO with a Faradaic efficiency over 95%. The partial current density reaches 452 mA cm−2 with approximately 91% CO Faradaic efficiency, and negligible C2+ products are observed. In situ spectroscopic measurements and theoretical simulations reason that the atomic Sb-Cu interface in Cu promotes CO2 adsorption/activation and weakens the binding strength of CO*, which ends up with enhanced CO selectivity and production rates.

Date: 2023
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DOI: 10.1038/s41467-023-35960-z

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