Catalyzing Desolvation at Cathode‐Electrolyte Interface Enabling High‐Performance Magnesium‐Ion Batteries

Magnesium ion batteries (MIBs) are expected to be the promising candidates in the post-lithium-ion era with high safety, low cost and almost dendrite-free nature. However, the sluggish diffusion kinetics and strong solvation capability of the strongly polarized Mg²⁺ are seriously limiting the specific capacity and lifespan of MIBs. In this work, catalytic desolvation is introduced into MIBs for the first time by modifying vanadium pentoxide (V₂O₅) with molybdenum disulfide quantum dots (MQDs), and it is demonstrated via density function theory (DFT) calculations that MQDs can effectively lower the desolvation energy barrier of Mg²⁺, and therefore catalyze the dissociation of Mg²⁺-1,2-Dimethoxyethane (Mg²⁺-DME) bonds and release free electrolyte cations, finally contributing to a fast diffusion kinetics within the cathode. Meanwhile, the local interlayer expansion can also increase the layer spacing of V₂O₅ and speed up the magnesiation/demagnesiation kinetics. Benefiting from the structural configuration, MIBs exhibit superb reversible capacity (≈300 mAh g^-1 at 50 mA g^-1) and unparalleled cycling stability (15 000 cycles at 2 A g^-1 with a capacity of ≈70 mAh g^-1). This approach based on catalytic reactions to regulate the desolvation behavior of the whole interface provides a new idea and reference for the development of high-performance MIBs.