Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction

Sheng-Chih Lin, Chun-Chih Chang, Shih-Yun Chiu, Hsiao-Tien Pai, Tzu-Yu Liao, Chia-Shuo Hsu, Wei-Hung Chiang, Ming-Kang Tsai () and Hao Ming Chen ()
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Sheng-Chih Lin: National Taiwan University
Chun-Chih Chang: Department of Chemical and Material Engineering, Chinese Culture University
Shih-Yun Chiu: National Taiwan University
Hsiao-Tien Pai: National Taiwan Normal University
Tzu-Yu Liao: National Taiwan University
Chia-Shuo Hsu: National Taiwan University
Wei-Hung Chiang: National Taiwan University of Science and Technology
Ming-Kang Tsai: National Taiwan Normal University
Hao Ming Chen: National Taiwan University

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract Copper electrocatalysts have been shown to selectively reduce carbon dioxide to hydrocarbons. Nevertheless, the absence of a systematic study based on time-resolved spectroscopy renders the functional agent—either metallic or oxidative Copper—for the selectivity still undecidable. Herein, we develop an operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts. An oxide-derived Copper electrocatalyst is employed as a model catalyst to offer scientific insights into the roles metal states serve in carbon dioxide reduction reaction (CO2RR). Using a potential switching approach, the model catalyst can achieve a steady chemical state of half-Cu(0)-and-half-Cu(I) and selectively produce asymmetric C2 products - C2H5OH. Furthermore, a theoretical analysis reveals that a surface composed of Cu-Cu(I) ensembles can have dual carbon monoxide molecules coupled asymmetrically, which potentially enhances the catalyst’s CO2RR product selectivity toward C2 products. Our results offer understandings of the fundamental chemical states and insights to the establishment of selective CO2RR.

Date: 2020
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DOI: 10.1038/s41467-020-17231-3

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