H‐/dT‐MoS2‐on‐MXene Heterostructures as Promising 2D Anode Materials for Lithium‐Ion Batteries: Insights from First Principles

Abstract

AbstractExperimental synthesis of two‐dimensional MoS2‐on‐MXene heterostructures and phase control of MoS2 have been demonstrated recently. Here, the electronic, electrochemical, mechanical properties, and structural morphology of MoS2@Ti2C and MoS2@Ti2CO2 heterostructures as anode materials for lithium‐ion batteries are systematically investigated by taking advantages of van der Waals corrected spin‐polarized density functional theory to give atomistic insights. The results herein demonstrate that, for the MoS2@Ti2CO2 heterostructure, MoS2 polymorph drastically affects the electronic structure and lithium (Li) diffusion at the interface. Li diffusion barrier at the interface of dT‐MoS2@Ti2CO2 along zigzag direction (0.15 eV) is much smaller than that of H‐MoS2@Ti2CO2 (0.67 eV). For the MoS2@Ti2C heterostructure, however, the Li diffusion behavior and electronic structure are relatively insensitive to MoS2 morphology. Especially, the MoS2@Ti2C heterostructures shows ultralow diffusion barrier, high charge–discharge rate, very low open‐circuit voltage (0.62–0.25 V), and high mechanical flexibility. These results suggest that MoS2@MXene heterostructures are promising anode materials for lithium‐ion batteries.