The nature of active sites for carbon dioxide electroreduction over oxide-derived copper catalysts

Dongfang Cheng, Zhi-Jian Zhao, Gong Zhang, Piaoping Yang, Lulu Li, Hui Gao, Sihang Liu, Xin Chang, Sai Chen, Tuo Wang, Geoffrey A. Ozin, Zhipan Liu and Jinlong Gong ()
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Dongfang Cheng: Tianjin University
Zhi-Jian Zhao: Tianjin University
Gong Zhang: Tianjin University
Piaoping Yang: Tianjin University
Lulu Li: Tianjin University
Hui Gao: Tianjin University
Sihang Liu: Tianjin University
Xin Chang: Tianjin University
Sai Chen: Tianjin University
Tuo Wang: Tianjin University
Geoffrey A. Ozin: University of Toronto
Zhipan Liu: Fudan University
Jinlong Gong: Tianjin University

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract The active sites for CO2 electroreduction (CO2R) to multi-carbon (C2+) products over oxide-derived copper (OD-Cu) catalysts are under long-term intense debate. This paper describes the atomic structure motifs for product-specific active sites on OD-Cu catalysts in CO2R. Herein, we describe realistic OD-Cu surface models by simulating the oxide-derived process via the molecular dynamic simulation with neural network (NN) potential. After the analysis of over 150 surface sites through NN potential based high-throughput testing, coupled with density functional theory calculations, three square-like sites for C–C coupling are identified. Among them, Σ3 grain boundary like planar-square sites and convex-square sites are responsible for ethylene production while step-square sites, i.e. n(111) × (100), favor alcohols generation, due to the geometric effect for stabilizing acetaldehyde intermediates and destabilizing Cu–O interactions, which are quantitatively demonstrated by combined theoretical and experimental results. This finding provides fundamental insights into the origin of activity and selectivity over Cu-based catalysts and illustrates the value of our research framework in identifying active sites for complex heterogeneous catalysts.

Date: 2021
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DOI: 10.1038/s41467-020-20615-0

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