Differentiating Contributions to “Ion Transfer” Barrier from Interphasial Resistance and Li⁺ Desolvation at Electrolyte/Graphite Interface

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Efforts were made to differentiate the contributions to the so-called "ion transfer" barrier at the electrolyte/graphite junction from two distinct processes: (1) desolvation of Li(+) before it enters graphene interlayer and (2) the subsequent migration of bare Li(+) through the ad hoc interphase. By leveraging a scenario where no substantial interphase was formed on Li(+) intercalation hosts, we were able to quantify the distribution of "ion transfer" activation energy between these two interfacial processes and hence identify the desolvation process of Li(+) as the major energy-consuming step. The result confirmed the earlier belief that the rate-determining step in the charging of a graphitic anode in Li(+) intercalation chemistry relates to the stripping of solvation sheath of Li(+), which is closely interwoven with the interphasial resistance to Li(+) migration.