Enabling Ultrafast Single Mg²⁺ Insertion Kinetics of Magnesium-Ion Batteries via In Situ Dynamic Catalysis and Re-equilibration Effects

Magnesium-ion batteries (MIBs) have great potential in large-scale energy storage field with high capacity, excellent safety, and low cost. However, the strong solvation effect of Mg 2+ will lead to the formation of solvated ions in electrolytes with larger size and sluggish diffusion/reaction kinetics. Here, the concept of interfacial catalytic bond breaking is first introduced into the cathode design of MIBs by hybriding MoS 2 quantum dots with VS 4 (VS 4 @MQDs) as the cathode. The “in situ dynamic catalysis and re-equilibration” effects can catalyze the Cl–Mg bond breaking and trigger single Mg 2+ insertion/extraction chemistries, which can significantly accelerate the diffusion and reaction kinetics, as verified by the decreased diffusion energy barriers (0.26 eV for Mg 2+ vs 2.47 eV for MgCl + ) and fast diffusion coefficient. Benefitting from these dynamic catalysis effects, the constructed VS 4 @MQD-based MIBs deliver a high discharge capacity of ∼120 mA h g –1 at 200 mA g –1 and a long-term cyclic stability of 1000 cycles at 1 A g –1 . The improved performance and detailed characterizations well prove that the active ions in MIBs change from MgCl + /Mg 2 Cl 3+ to Mg 2+ with fast kinetics.