Kinetics of the CO 2 reduction reaction in aprotic Li–CO 2 batteries: a model study

The aprotic Li–CO 2 battery represents a promising technology that can potentially achieve energy conversion and storage and CO 2 recycling simultaneously. However, current Li–CO 2 batteries suffer from the sluggish kinetics of the CO 2 reduction reaction (CO 2 RR) which often leads to high discharg...

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Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2021-02, Vol.9 (6), p.3290-3296
Main Authors: Zhao, Zhiwei, Wang, Erkang, Wang, Jiawei, Liu, Chuntai, Peng, Zhangquan
Format: Article
Language:English
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Summary:The aprotic Li–CO 2 battery represents a promising technology that can potentially achieve energy conversion and storage and CO 2 recycling simultaneously. However, current Li–CO 2 batteries suffer from the sluggish kinetics of the CO 2 reduction reaction (CO 2 RR) which often leads to high discharge overpotential, low energy efficiency, and low power densities. Toward unlocking the energy capabilities of Li–CO 2 batteries, it is crucially important to have a fundamental understanding of the kinetics aspect of the Li–CO 2 electrochemistry. Here we report a brief but comprehensive model to bridge the overall reaction kinetics and the elementary steps of the CO 2 RR in Li–CO 2 batteries. A critical kinetics descriptor, i.e. , the adsorption energy of the LiCO 2 intermediate on the cathode surface, is proposed to reveal the interplay and competition between two different CO 2 RR mechanisms ( i.e. , the solution- and the surface-mediated pathways) occurring in Li–CO 2 batteries. Our model indicates that tuning the CO 2 RR toward the solution-mediated pathway can avoid cathode surface passivation and is favorable for high-capacity and high-rate discharging of Li–CO 2 batteries. The model study reported here sheds light on the kinetics aspect of Li–CO 2 electrochemistry and would be beneficial for the design of better Li–CO 2 batteries.
ISSN:2050-7488
2050-7496
DOI:10.1039/D0TA11281J