Theoretical evaluation of monolayer MAZ (M = Ti, Zr, or Hf; A = Si or Ge; and Z = P or As) family as promising candidates for lithium-sulfur batteries.

Rechargeable lithium-sulfur (Li-S) batteries have been considered as a potential energy storage system due to their high theoretical specific energy. However, their practical commercial application has been hindered by unresolved key issues. One promising approach to overcoming these challenges is the development of anchoring materials with exceptional performance. In this work, we conducted detailed evaluations of twelve types of MAZ (M = Ti, Zr, or Hf; A = Si or Ge; and Z = P or As) monolayers as potential Li-S battery electrodes through first-principles calculations. Our results indicate that these monolayers can effectively immobilize LiS species, preventing them from dissolving into the electrolyte and preserving intact LiS conformations. The high electrical conductivity of these monolayers can be perfectly retained after S/LS clusters adsorption. Furthermore, the MAP monolayers demonstrate superior catalytic performance for the sulfur reduction reaction (SRR) compared to the MAAs counterparts, whereas the MAAs monolayers exhibit lower decomposition energy barriers. Our current work indicates that these MAZ monolayers hold significant promise as electrode materials for Li-S batteries.