Control of Electrolyte\nDesolvation Energy Suppressing\nthe Cointercalation Mechanism and Organic Electrode Dissolution

Despite numerous studies aimed at solving the detrimental\ndissolution\nissue of organic electrode materials (OEMs), a fundamental understanding\nof their dissolution mechanism has not yet been established. Herein,\nwe systematically investigate how changes in electrolyte composition\naffect the ion-solvent interactions propagating to OEM dissolution\nby changing the cation. The cyclability of OEM is significantly different\nby alkali cations, where the OEM with K is stable even after 300 cycles\nand that with Li is drastically decayed within 100 cycles. This different\nbehavior is owing to the dissolution of OEM into electrolytes, and\nthe dissolution of OEMs was found to be highly dependent on the cation-solvent\ninteraction. Strong cation-solvent interactions induce cointercalation\ninto the layered structure of the electrode and cause electrode deformation.\nThis behavior allows OEMs to easily detach from their original location,\nconsequently leading to dissolution and severe capacity decay. The\ncation-solvent interaction-dependent phenomenon is similar to that\nof OEMs with high-concentration electrolytes, in which fewer cation-solvent\npairs exist. The result provides insight into proper electrolyte selection\nand is expected to set a constructive milestone in the utilization\nof organic electrodes.