Activated Co in Thiospinel Boosting Li<sub>2</sub>CO<sub>3</sub> Decomposition in Li−CO<sub>2</sub> Batteries
Yanli Chen, Junfeng Li, Bingyi Lu, Yingqi Liu, Rui Mao, Yanze Song, Hongtai Li, Xinqian Yu, Yongzheng Gao, Qiong Peng, Xiaosi Qi, Guangmin Zhou
Abstract
Abstract Catalytic reactions mainly depend on the adsorption properties of reactants on the catalyst, which provides a perspective for the design of reversible lithium−carbon dioxide (Li−CO 2 ) batteries including CO 2 reduction (CO 2 RR) and CO 2 evolution (CO 2 ER) reactions. However, due to the complex reaction process, the relationship between the adsorption configuration and CO 2 RR/CO 2 ER catalytic activity is still unclear in Li ─ CO 2 batteries. Herein, taking Co 3 S 4 as a model system, nickel (Ni substitution in the tetrahedral site to activate cobalt (Co) atom for forming multiatom catalytic domains in NiCo 2 S 4 is utilized. Benefiting from the special geometric and electronic structures, NiCo 2 S 4 exhibits an optimized adsorption configuration of lithium carbonate (Li 2 CO 3 ), promoting its effective activation and decomposition. As a result, the Li−CO 2 batteries with NiCo 2 S 4 cathode exhibit remarkable electrochemical performance in terms of low potential gap of 0.42 V and high energy efficiency of 88.7%. This work provides a unique perspective for the development of highly efficient catalysts in Li−CO 2 batteries.