Stable multi-electron reaction stimulated by W doping VS4 for enhancing magnesium storage performance

Rechargeable magnesium batteries (RMBs) hold promise for offering higher volumetric energy density and safety features, attracting increasing research interest as the next post lithium-ion batteries. Developing high performance cathode material by inducing multi-electron reaction process as well as maintaining structural stability is the key to the development and application of RMBs. Herein, multi-electron reaction occurred in VS₄ by simple W doping strategy. W doping induces valence of partial V as V²⁺ and V³⁺ in VS₄ structure, and then stimulates electrochemical reaction involving multi-electrons in 0.5% W-V-S. The flower-like microsphere morphology as well as rich S vacancies is also modulated by W doping to neutralize structure change in such multi-electron reaction process. The fabricated 0.5% W-V-S delivers higher specific capacity (149.3 mA h g⁻¹ at 50 mA g⁻¹, which is 1.6 times higher than that of VS₄), superior rate capability (76 mA h g⁻¹ at 1000 mA g⁻¹), and stable cycling performance (1500 cycles with capacity retention ratio of 93.8%). Besides that, pesudocapaticance-like contribution analysis as well as galvanostatic intermittent titration technique (GITT) further confirms the enhanced Mg²⁺ storage kinetics during such multi-electron involved electrochemical reaction process. Such discovery provides new insights into the designing of multi-electron reaction process in cathode as well as neutralizing structural change during such reaction for realizing superior electrochemical performance in energy storage devices.