Phase transition and electrochemical properties of S-functionalized MXene anodes for Li-ion batteries: a first-principles investigation.

The advancement of anode materials for achieving high energy storage is a crucial topic for high-performance Li-ion batteries (LIBs). Here, first-principles calculations were used to conduct a thorough and systematic investigation into lithium storage properties of MXenes with new S functional groups as LIB anode materials. Density of states, diffusion energy barriers, open circuit voltages and storage capacities were calculated to comprehensively evaluate the lithium storage properties of S-functionalized MXenes. Based on the computational results, Ti 2 CS 2 and V 2 CS 2 were selected as excellent candidates from ten M 2 CS 2 MXenes. The diffusion energy barriers of M 2 CS 2 within the range of 0.26-0.32 eV are lower than those of M 2 CO 2 and M 2 CF 2 , indicating that M 2 CS 2 anodes exhibit faster charge/discharge rates. By examining the stable crystal structures and comparing atomic positions before and after Li adsorptions, structural phase transitions during Li-ion adsorptions could happen for nearly all M 2 CS 2 MXenes. The phase transitions predicted were directly observed using ab initio molecular dynamic simulations. The cycle stability, storage capacity and other lithium storage properties were enhanced by the reversible structural phase transition.