Theoretical Exploration of a High-Entropy Transformation Strategy for Li-SO₂Cl₂ Reserve Battery Electrolytes

High-entropy transformation of the electrolyte is a cutting-edge strategy to improve the comprehensive performance of traditional electrolytes. High-entropy electrolytes (HEEs) represent a paradigm shift in battery electrolyte design. Especially, for Li-SO₂Cl₂ reserve chemical batteries, the high-entropy transformation of SO₂Cl₂ electrolytes is worthwhile to explore. Different from the conventional method of mixing multiple solvent components, a high-entropy transformation of the electrolyte is proposed by introducing active species with a structure similar to the original electrolyte but with unique properties as "spy molecules" into the aggregate network of the original electrolyte molecules. Namely, the high-entropy key component, CrO₂Cl₂ (spy molecule), is suggested as a reasonable additive for the SO₂Cl₂ electrolyte, in which CrO₂Cl₂ is precisely the "spy molecules." For this purpose, the potential application and feasibility are explored based on theoretical calculations from the analysis of several aspects, including the geometric configurations and intermolecular interactions, vertical electron affinity and adiabatic electron affinity, thermodynamic and kinetic analysis of CrO₂Cl₂ reduction, and the standard electrode potential of the CrO₂Cl₂/³[CrO₂Cl]^- electrode pair.