Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol

Xiaozhi Su, Zhuoli Jiang, Jing Zhou, Hengjie Liu, Danni Zhou, Huishan Shang, Xingming Ni, Zheng Peng, Fan Yang, Wenxing Chen (), Zeming Qi, Dingsheng Wang and Yu Wang ()
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Xiaozhi Su: Chinese Academy of Sciences
Zhuoli Jiang: Beijing Institute of Technology
Jing Zhou: Chinese Academy of Sciences
Hengjie Liu: University of Science and Technology of China
Danni Zhou: Beijing Institute of Technology
Huishan Shang: Beijing Institute of Technology
Xingming Ni: ShanghaiTech University
Zheng Peng: ShanghaiTech University
Fan Yang: ShanghaiTech University
Wenxing Chen: Beijing Institute of Technology
Zeming Qi: University of Science and Technology of China
Dingsheng Wang: Tsinghua University
Yu Wang: Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity. The atomic structure-activity relationship of electrocatalysts for the selectivity is controversial due to the lacking of systemic multiple dimensions for operando condition study. Herein, we synthesized high-performance CO2RR catalyst comprising of CuO clusters supported on N-doped carbon nanosheets, which exhibited high C2+ products Faradaic efficiency of 73% including decent ethanol selectivity of 51% with a partial current density of 14.4 mA/cm−2 at −1.1 V vs. RHE. We evidenced catalyst restructuring and tracked the variation of the active states under reaction conditions, presenting the atomic structure-activity relationship of this catalyst. Operando XAS, XANES simulations and Quasi-in-situ XPS analyses identified a reversible potential-dependent transformation from dispersed CuO clusters to Cu2-CuN3 clusters which are the optimal sites. This cluster can’t exist without the applied potential. The N-doping dispersed the reduced Cun clusters uniformly and maintained excellent stability and high activity with adjusting the charge distribution between the Cu atoms and N-doped carbon interface. By combining Operando FTIR and DFT calculations, it was recognized that the Cu2-CuN3 clusters displayed charge-asymmetric sites which were intensified by CH3* adsorbing, beneficial to the formation of the high-efficiency asymmetric ethanol.

Date: 2022
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DOI: 10.1038/s41467-022-29035-8

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