ABSTRACT Magnesium batteries are compelling post‐lithium energy storage candidates but suffer from sluggish charge transfer kinetics, fundamentally restricted by the high energy barrier of Mg 2+ desolvation. Herein, we address the compact and tenacious solvation sheath induced by the high charge density of Mg 2+ , characterized by strong electrostatic binding. To effectively weaken the coordination strength and lower the desolvation barrier, we utilize machine learning to identify electrolytes that energetically balance Mg 2+ ‐solvent and Mg 2+ ‐anion interactions. This counterpoise state leads to a comprehensive weakening of the solvation shell. As corroborated by in situ Raman spectroscopy, this environment facilitates a synchronous desolvation pathway and induces a robust MgH 2 ‐based solid‐electrolyte interphase, fundamentally accelerating interfacial kinetics. The screened amine‐based electrolyte empowers low‐overpotential Mg 2+ reduction of 0.06 V at 1 mA cm −2 , and full cells with high‐rate performance sustain 50 C cycling, and a Mg/fluorinated carbon cell delivers 918 mAh g −1 at 0.5 C. This paradigm shifts the design focus from individual solvation to collective energy equilibration in multivalent electrolytes.
Zhang et al. (Fri,) studied this question.