Citation: Jianing Mao, Bingbao Mei, Ji Li, Shuai Yang, Fanfei Sun, Siyu Lu, Wei Chen, Fei Song, Zheng Jiang. Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO₂ Electroreduction[J]. Chinese Journal of Structural Chemistry, ;2022, 41(10): 221008. doi: 10.14102/j.cnki.0254-5861.2022-0133 shu

Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO₂ Electroreduction

Jianing Mao ^{1, 2, 3} ,
Bingbao Mei ^{2, 3,,} ,
Ji Li ^{1, 2, 3} ,
Shuai Yang ^{1, 2, 3} ,
Fanfei Sun ^{2, 3} ,
Siyu Lu ⁴ ,
Wei Chen ^{2, 5} ,
Fei Song ^{1, 2, 3,,} ,
Zheng Jiang ^{1, 2, 3, 6,,}

1.
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China
4.
College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450000, China
5.
Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Science, Shanghai 201210, China
6.
Innovation Academy for Green Manufacture, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Bingbao Mei, meibb@sari.ac.cn Fei Song, songfei@sinap.ac.cn Zheng Jiang, jiangzheng@sinap.ac.cn
Received Date: 21 May 2022
Accepted Date: 2 June 2022
Available Online: 8 June 2022

Figures(4)

Understanding the atomic and electronic changes of active sites promotes the whole new sight into electrochemical carbon dioxide reduction reaction (CO₂RR), which provides a feasible strategy to achieve carbon neutrality. Here we employ operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy (HERFD-XAS) to track the structural evolution of Ni(II) phthalocyanine (NiPc), considered as the model catalysts with uniform Ni-N₄-C₈ moiety, during the CO₂RR. The HERFD-XAS method is in favor of elucidating the interaction of the reactant/catalyst interface from the atomic electronic structure dimension, facilitating the establishment of the catalytic mechanism and the dynamic structure changes. Based on operando measurement, surface sensitive difference spectra (∆µ) and spectroscopy simulation, the interfacial interactions between the active sites of NiPc and reactants are monitored and the Ni species gradually reduced by increasing the applied potential is discovered. HERFD-XAS method offers an advanced and powerful tool for elucidating the complex catalytic mechanism in further various systems.
- CO₂ electrochemical reduction,
- HERFD-XAS,
- model catalysts,
- difference spectra,
- structural evolution
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Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO2 Electroreduction

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通讯作者: 陈斌, bchen63@163.com

Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO₂ Electroreduction