Mechanistic insights into C-C coupling in electrochemical CO reduction using gold superlattices

Xiaoju Yang, Chao Rong, Li Zhang, Zhenkun Ye, Zhiming Wei, Chengdi Huang, Qiao Zhang, Qing Yuan, Yueming Zhai, Fu-Zhen Xuan, Bingjun Xu (), Bowei Zhang () and Xuan Yang ()
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Xiaoju Yang: Huazhong University of Science and Technology
Chao Rong: East China University of Science and Technology
Li Zhang: Huazhong University of Science and Technology
Zhenkun Ye: Huazhong University of Science and Technology
Zhiming Wei: Wuhan University
Chengdi Huang: Huazhong University of Science and Technology
Qiao Zhang: Wuhan University
Qing Yuan: Huazhong University of Science and Technology
Yueming Zhai: Wuhan University
Fu-Zhen Xuan: East China University of Science and Technology
Bingjun Xu: Peking University
Bowei Zhang: East China University of Science and Technology
Xuan Yang: Huazhong University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Developing in situ/operando spectroscopic techniques with high sensitivity and reproducibility is of great importance for mechanistic investigations of surface-mediated electrochemical reactions. Herein, we report the fabrication of highly ordered rhombic gold nanocube superlattices (GNSs) as substrates for surface-enhanced infrared absorption spectroscopy (SEIRAS) with significantly enhanced SEIRA effect, which can be controlled by manipulating the randomness of GNSs. Finite difference time domain simulations reveal that the electromagnetic effect accounts for the significantly improved spectroscopic vibrations on the GNSs. In situ SEIRAS results show that the vibrations of CO on the Cu2O surfaces have been enhanced by 2.4 ± 0.5 and 18.0 ± 1.3 times using GNSs as substrates compared to those on traditional chemically deposited gold films in acidic and neutral electrolytes, respectively. Combined with isotopic labeling experiments, the reaction mechanisms for C-C coupling of CO electroreduction on Cu-based catalysts are revealed using the GNSs substrates.

Date: 2024
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DOI: 10.1038/s41467-024-44923-x

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