期刊
ACS ENERGY LETTERS
卷 7, 期 2, 页码 624-631出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c02773
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资金
- National Key R&D Program of China [2018YFB0104400]
- National Natural Science Foundation of China [21972055, 21825202, 21733012, 21972133, 92045302]
- Newton Advanced Fellowships [NAF/R2/180603]
This study provides new insights into the mechanism of CO2 reduction reaction (CO2RR) in Li-CO2 batteries through a combination of experimental and computational methods. A new discharge pathway is proposed based on the spectroscopic evidence obtained. The study also reveals the significant effect of the electrocatalysts' near-Fermi-level d-orbital states on the CO2RR activity. Additionally, the deep CO2RR process may be limited by sluggish chemical reactions.
The aprotic Li-CO2 battery represents a sustainable technology by virtue of energy storage capability and CO2 recyclability. However, the CO2 reduction reaction (CO2RR) mechanism underpinning the operation of Li-CO2 batteries is not yet completely understood. Herein, using in situ surface-enhanced Raman spectroscopy coupled with density functional theory calculations, we obtain direct spectroscopic evidence of the CO2RR (i.e., CO2-, CO, and Li2CO3) and propose a surface-mediated discharge pathway (i.e., 2Li(+) + 2CO(2) + 2e(-) -> CO + Li2CO3) in Li-CO2 batteries. We also highlight the significant effect of the electrocatalysts' near-Fermi-level d-orbital states on the CO2RR activity through a systematic comparative study of model electrocatalysts. Moreover, deep CO2RR via 4Li(+) + 3CO(2) + 4e(-) -> 2Li(2)CO(3) + C may be difficult to proceed because of the sluggish chemical steps involved (e.g., dimerization of two CO2- intermediates). This work provides molecular insights into the CO2RR mechanism in a Li+-aprotic medium and will be beneficial for nextgeneration Li-CO2 batteries.
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