Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion

Yangyang Zhang, Yanxu Chen, Xiaowen Wang, Yafei Feng, Zechuan Dai, Mingyu Cheng and Genqiang Zhang ()
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Yangyang Zhang: University of Science and Technology of China
Yanxu Chen: University of Science and Technology of China
Xiaowen Wang: University of Science and Technology of China
Yafei Feng: University of Science and Technology of China
Zechuan Dai: University of Science and Technology of China
Mingyu Cheng: University of Science and Technology of China
Genqiang Zhang: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The carbon−carbon coupling at the Cu/Cu2O Schottky interface has been widely recognized as a promising approach for electrocatalytic CO2 conversion into value-added alcohols. However, the limited selectivity of C2+ alcohols persists due to the insufficient control over rectifying interface characteristics required for precise bonding of oxyhydrocarbons. Herein, we present an investigation into the manipulation of the coordination environment of Cu sites through an in-situ electrochemical reconstruction strategy, which indicates that the construction of low-coordinated Cu sites at the Cu/Cu2O interface facilitates the enhanced rectifying interfaces, and induces asymmetric electronic perturbation and faster electron exchange, thereby boosting C-C coupling and bonding oxyhydrocarbons towards the nucleophilic reaction process of *H2CCO-CO. Impressively, the low-coordinated Cu sites at the Cu/Cu2O interface exhibit superior faradic efficiency of 64.15 ± 1.92% and energy efficiency of ~39.32% for C2+ alcohols production, while maintaining stability for over 50 h (faradic efficiency >50%, total current density = 200 mA cm−2) in a flow-cell electrolyzer. Theoretical calculations, operando synchrotron radiation Fourier transform infrared spectroscopy, and Raman experiments decipher that the low-coordinated Cu sites at the Cu/Cu2O interface can enhance the coverage of *CO and adsorption of *CH2CO and CH2CHO, facilitating the formation of C2+ alcohols.

Date: 2024
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DOI: 10.1038/s41467-024-49247-4

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