Stability and Performance of 3d Transition Metal Carbo‐Sulfides: A Density Functional Theory Exploration for Li‐Ion Battery Anodes

Abstract

As the demand for high-performance and reliable energy storage devices continues to rise, identifying new anode materials is crucial for advancing Li-ion battery (LIB) technology. Inspired by recent experimental breakthroughs in synthesizing two-dimensional transition metal carbo-chalcogenides (2D-TMCCs), density functional theory calculations are performed to systematically explore their sulfide variants (TM 2 S 2 C) spanning all 3d transition metals in three possible phases. Through comprehensive evaluations of thermodynamic, dynamic, mechanical, and thermal stabilities, seven stable 2D-TMCC candidates are identified, four of which exhibit superior battery performance. Notably, V-based 2D-TMCCs across all three phases deliver moderate open-circuit voltages (OCV), efficient Li diffusion, and substantial capacities, making them promising candidates for industrial applications without requiring specific phase controls. A Cr-based 2D-TMCC (with sulfur atoms above carbon atoms) offers the highest capacity of 515.40 mAh g −1 , the lowest Li diffusion barrier, and an optimal OCV, highlighting its appealing potential as an anode material for LIBs. Furthermore, significant Li–Li spacing and pronounced electron delocalization in these four 2D-TMCCs suggest a reduced risk of dendrite formation. This work expands the 2D-TMCC family and identifies up-and-coming candidates for next-generation LIB anodes.