Improving CO2 photoconversion with ionic liquid and Co single atoms

Yang Liu; Jianhui Sun; Houhou Huang; Linlu Bai; Xiaomeng Zhao; Binhong Qu; Lunqiao Xiong; Fuquan Bai; Junwang Tang; Liqiang Jing

doi:10.1038/s41467-023-36980-5

Improving CO₂ photoconversion with ionic liquid and Co single atoms

Nat Commun. 2023 Mar 16;14(1):1457. doi: 10.1038/s41467-023-36980-5.

Authors

Yang Liu^#¹, Jianhui Sun^#^{1

2}, Houhou Huang³, Linlu Bai⁴, Xiaomeng Zhao¹, Binhong Qu¹, Lunqiao Xiong⁵, Fuquan Bai³, Junwang Tang⁶, Liqiang Jing⁷

Affiliations

¹ Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Heilongjiang University, Harbin, Heilongjiang, 150080, P. R. China.
² Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), International Joint Research Center for Catalytic Technology, School of Physics, Heilongjiang University, Harbin, 150080, P. R. China.
³ International Joint Research Laboratory of Nano-Micro Architecture Chemistry, Institute of Theoretical Chemistry and College of Chemistry, Jilin University Changchun, 130021, Changchun, P. R. China.
⁴ Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Heilongjiang University, Harbin, Heilongjiang, 150080, P. R. China. llbai@hlju.edu.cn.
⁵ Department of Chemical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK.
⁶ Department of Chemical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK. junwang.tang@ucl.ac.uk.
⁷ Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Heilongjiang University, Harbin, Heilongjiang, 150080, P. R. China. jinglq@hlju.edu.cn.

^# Contributed equally.

Abstract

Photocatalytic CO₂ conversion promises an ideal route to store solar energy into chemical bonds. However, sluggish electron kinetics and unfavorable product selectivity remain unresolved challenges. Here, an ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate, and borate-anchored Co single atoms were separately loaded on ultrathin g-C₃N₄ nanosheets. The optimized nanocomposite photocatalyst produces CO and CH₄ from CO₂ and water under UV-vis light irradiation, exhibiting a 42-fold photoactivity enhancement compared with g-C₃N₄ and nearly 100% selectivity towards CO₂ reduction. Experimental and theoretical results reveal that the ionic liquid extracts electrons and facilitates CO₂ reduction, whereas Co single atoms trap holes and catalyze water oxidation. More importantly, the maximum electron transfer efficiency for CO₂ photoreduction, as measured with in-situ μs-transient absorption spectroscopy, is found to be 35.3%, owing to the combined effect of the ionic liquid and Co single atoms. This work offers a feasible strategy for efficiently converting CO₂ to valuable chemicals.

Abstract

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