Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy

Li Zhang; Xiaoju Yang; Qing Yuan; Zhiming Wei; Jie Ding; Tianshu Chu; Chao Rong; Qiao Zhang; Zhenkun Ye; Fu-Zhen Xuan; Yueming Zhai; Bowei Zhang; Xuan Yang

doi:10.1038/s41467-023-44078-1

Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy

Nat Commun. 2023 Dec 14;14(1):8311. doi: 10.1038/s41467-023-44078-1.

Authors

Li Zhang^{1

2}, Xiaoju Yang^{1

2}, Qing Yuan^{1

2}, Zhiming Wei³, Jie Ding³, Tianshu Chu⁴, Chao Rong⁴, Qiao Zhang³, Zhenkun Ye^{1

2}, Fu-Zhen Xuan⁴, Yueming Zhai³, Bowei Zhang⁵, Xuan Yang^{6

7}

Affiliations

¹ Key Laboratory of Material Chemistry for Energy Conversion and Storage, Huazhong University of Science and Technology, Wuhan, 430074, China.
² Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China.
³ The Institute for Advanced Studies, Wuhan University, Wuhan, 430072, China.
⁴ Shanghai Key Laboratory of Intelligent Sensing and Detection Technology, Key Laboratory of Pressure Systems and Safety of Ministry of Education, School of Mechanical and Power Engineering, East China University of Science and Technology, Shanghai, 200237, China.
⁵ Shanghai Key Laboratory of Intelligent Sensing and Detection Technology, Key Laboratory of Pressure Systems and Safety of Ministry of Education, School of Mechanical and Power Engineering, East China University of Science and Technology, Shanghai, 200237, China. boweiz@ecust.edu.cn.
⁶ Key Laboratory of Material Chemistry for Energy Conversion and Storage, Huazhong University of Science and Technology, Wuhan, 430074, China. xuanyang@hust.edu.cn.
⁷ Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China. xuanyang@hust.edu.cn.

Abstract

Understanding the structure-stability relationship of catalysts is imperative for the development of high-performance electrocatalytic devices. Herein, we utilize operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to quantitatively monitor the evolution of Cu single-atom catalysts (SACs) during the electrochemical reduction of CO₂ (CO₂RR). Cu SACs are converted into 2-nm Cu nanoparticles through a reconstruction process during CO₂RR. The evolution rate of Cu SACs is highly dependent on the substrates of the catalysts due to the coordination difference. Density functional theory calculations demonstrate that the stability of Cu SACs is highly dependent on their formation energy, which can be manipulated by controlling the affinity between Cu sites and substrates. This work highlights the use of operando ATR-SEIRAS to achieve mechanistic understanding of structure-stability relationship for long-term applications.