Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption

Xin Chen, Junxiang Chen, Huayu Chen, Qiqi Zhang, Jiaxuan Li, Jiwei Cui, Yanhui Sun, Defa Wang, Jinhua Ye and Lequan Liu ()
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Xin Chen: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Junxiang Chen: Chinese Academy of Sciences
Huayu Chen: China Jiliang University
Qiqi Zhang: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Jiaxuan Li: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Jiwei Cui: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Yanhui Sun: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Defa Wang: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Jinhua Ye: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University
Lequan Liu: Key Lab of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Exploring efficient electrocatalysts with fundamental understanding of the reaction mechanism is imperative in CO2 electroreduction. However, the impact of sluggish water dissociation as proton source and the surface species in reaction are still unclear. Herein, we report a strategy of promoting protonation in CO2 electroreduction by implementing oxygen vacancy engineering on Bi2O2CO3 over which high Faradaic efficiency of formate (above 90%) and large partial current density (162 mA cm−2) are achieved. Systematic study reveals that the production rate of formate is mainly hampered by water dissociation, while the introduction of oxygen vacancy accelerates water dissociation kinetics by strengthening hydroxyl adsorption and reduces the energetic span of CO2 electroreduction. Moreover, CO3* involved in formate formation as the key surface species is clearly identified by electron spin resonance measurements and designed in situ Raman spectroscopy study combined with isotopic labelling. Coupled with photovoltaic device, the solar to formate energy conversion efficiency reaches as high as 13.3%.

Date: 2023
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DOI: 10.1038/s41467-023-36263-z

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