Understanding the Anchoring and Catalytic Effect of the Co@CN Monolayer in Lithium-selenium Batteries: a First-principles Study

The practical applications of lithium-selenium (Li-Se) batteries are impeded due to the low utilization of active selenium, sluggish kinetics, and volume change. The development of highly efficient host materials to suppress high-order polyselenide shuttling and accelerate LiSe conversion is essential for Li-Se batteries. Herein, a theoretical design of a Co@CN monolayer as a host material for ultra-high areal capacity Li-Se batteries is proposed by first-principles calculations. The investigations of the lowest energy configurations, binding energies, and the charge transfer indicate that the Co@CN monolayer could alleviate the reciprocating motion of high-order polyselenides and improve the cycling performance. Further electronic property calculations show that the semi-metallic characteristics of the Co@CN monolayer material are retained even after chemical adsorption with Se or LiSe molecules, which is beneficial for the utilization of active selenium. In addition, the crucial catalytic role of the Co@CN monolayer is investigated and the results indicate that the Co@CN monolayer could facilitate the formation and decomposition of LiSe molecules during the discharge and charge processes. Our present work would not only provide a deep understanding on the anchoring and catalytic effect of the Co@CN monolayer, but also demonstrate a general principle for the rational design and screening of advanced materials for high energy density Li-Se batteries.