Homonuclear Transition-Metal Dimers Embedded Monolayer C2n as Promising Anchoring and Electrocatalytic Materials for Lithium-Sulfur Battery: First-Principles Calculations

Abstract

The practical applications of lithium-sulfur (Li-S) battery are greatly impeded by several bottlenecks, such as the dissolution of lithium polysulfides (LiPSs) and the poor conversion efficiency during discharging/charging processes . To handle these issues, we construct homonuclear transition-metal dimers embedded in monolayer C2N (TM2@C2N, TM = Cu, V, Co, Fe, and Ni) structures and comprehensively explore their potential as anchoring and electrocatalytic materials in Li-S battery by using first-principles calculations. It is found that the TM2@C2N have excellent anchoring ability for LiPSs with moderate adsorption energy, which can effectively suppress the shuttle effect. The introduction of TM dimer in monolayer C2N can reduce the free energy of sulfur reduction reaction to 1.22−1.46 eV and decrease the decomposition energy barriers of electrochemical conversions to 0.82−1.29 eV, which make the high activity to the catalytic conversion and the enhanced catalytic conversion efficiency in the discharging/charging processes. This work not only reveals that the TM2@C2N can serve as electrocatalysts to facilitate the adsorption for LiPSs and the catalytic conversion of the high-performance Li-S battery, but also provides a guidance for the homonuclear dual-atom catalysts design in Li-S battery.

Keywords: Lithium-sulfur battery, Dual-atom catalysts, First-principles calculations, cathode host materials