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[JACS] Prof. Jian-Feng Li published a paper entitled "Unveiling the Solvation Chemistry and Surface Effects on CO2 Reduction Reaction Pathways in Nonaqueous Li–CO2 Batteries"

Posted:2025-06-05  Visits:

Title: Unveiling the Solvation Chemistry and Surface Effects on CO2 Reduction Reaction Pathways in Nonaqueous Li–CO2 Batteries

Authors: Fan Gao, Mu-Fei Yue, Daniel Wun Fung Cheung, Weimin Yang, Zhi-Feng He, Yu Gu*, Shisheng Zheng*, Xiaobin Zhong, Siyuan Ma, Wei-Ping Chen, Jing-Hua Tian, Jin-Chao Dong*, Jian-Feng Li*

Abstract: Achieving highly reversible Li–CO2 batteries requires efficient and reversible CO2 redox reactions. However, the CO2 reduction reaction (CO2RR) mechanism during discharge in nonaqueous electrolytes, strongly influenced by the solvent environment and surface structure, remains unclear. Here, we systematically investigate the CO2RR on atomically flat Au(hkl) single crystal surfaces, providing direct spectral evidence of vital surface/intermediate species using in situ Raman spectroscopy. Our findings, combined with theoretical calculations, reveal that high-donor-number (DN) electrolytes facilitate a solution-mediated pathway, where Li+ forms stable solvation structures with solvent molecules that react with *CO2 to produce CO and Li2CO3. Conversely, low-DN electrolytes promote a surface-mediated pathway due to limited solvation, enhancing direct Li+–*CO2 interactions on the electrode surface. Among the various Au(hkl) surfaces, Au(110) shows superior catalytic activity, greatly enhancing *CO2 activation. This research offers crucial insights into the interplay between solvent chemistry and surface structure in the CO2RR, guiding future Li–CO2 batteries optimization.

Full-Link: https://pubs.acs.org/doi/10.1021/jacs.5c04157