Boosting reaction kinetics and reversibility in Mott-Schottky VS₂/MoS₂ heterojunctions for enhanced lithium storage

Heterostructures have lately been recognized as a viable implement to achieve high-energy Li-ion batteries (LIBs) because the as-formed built-in electric field can greatly accelerate the charge transfer kinetics. Herein, we have constructed the Mott-Schottky heterostructured VS₂/MoS₂ hybrids with tailorable 1T/2H phase based on their matchable formation energy, which are made of metallic and few-layered VS₂ vertically grown on MoS₂ surface. The density functional theory (DFT) calculations unveil that such heterojunctions drive the rearrangement of energy band with a facilitated reaction kinetics and enhance the Li adsorption energy more than twice compared to the MoS₂ surface. Furthermore, the VS₂ catalytically expedites the Li-S bond fracture and meantime the enriched Mo⁶⁺ enables the sulfur anchoring toward the oriented reaction with Li⁺ to form Li₂S, synergistically enhancing the reversibility of electrochemical redox. Consequently, the as-obtained VS₂/MoS₂ hybrids deliver a very large specific capacity of 1273 mAh g^-1 at 0.1 A g^-1 with 61% retention even at 5 A g^-1. It can also stabilize 100 cycles at 0.5 A g^-1 and 500 cycles at 1 A g^-1. The findings provide in-depth insights into engineering heterojunctions towards the enhancement of reaction kinetics and reversibility for LIBs.