Oxidized Kinetic Normal Distribution Models for Sophisticated Electrochemical Windows

Abstract

The electrochemical window (EW) of electrolytes is considered the essential bottleneck of the voltage range for lithium batteries, which is theoretically overestimated previously. In this work, we present an innovative strategy to quantify the EW without experiential parameters accurately. This strategy encompasses energy states and statistical distribution from both thermodynamic and oxidized kinetic aspects. Verified by linear sweep voltammetry, which specializes in intrinsic redox kinetics of reactants and excludes the influences of products, the most restrictive factor among the effects of condensation, thermal motion, solvent, electric field, and catalysis determines the practical EW. For polyethylene oxide (PEO) and ethylene carbonate (EC)-dimethyl carbonate (DMC) with glassy carbon, the solvent effect is the restriction, while for EC-DMC with LixCoO2, the catalysis effect of the LixCoO2 surface is the restriction. This work provides an effective criterion for accurate prediction, guiding the electrolyte system design to satisfy the expected EW.