Kinetics of Interfacial Ion Transfer in Lithium-Ion Batteries: Mechanism Understanding and Improvement Strategies

ACS Appl Mater Interfaces. 2022 Feb 15. doi: 10.1021/acsami.1c21683. Online ahead of print.

Abstract

The development of high-rate lithium-ion batteries is required for automobile applications. To this end, internal resistances must be reduced, among which Li+ transfer resistance at electrode/electrolyte interfaces is known to be the largest. Hence, it is of urgent significance to understand the mechanism and kinetics of the interfacial Li+ transfer. This Spotlight on Applications presents recent progress in the analysis and mechanical understanding of interfacial Li+ transfer. First, we review the reported activation energies (Ea) at various solid/liquid interfaces. On this basis, the mechanism and rate-determining step of the interfacial Li+ transfer are discussed from the viewpoints of the desolvation of Li+, the nature of the solid electrolyte interphase (SEI), and the surface structural features of electrodes. After that, we introduce promising strategies to reduce the Ea, highlighting some specific cases that give remarkably low Ea. We also note the variations in frequency factors or pre-exponential factors (A) of the interfacial Li+ transfer, which are primarily dominated by the number of Li+ intercalation sites on electrode surfaces. The current understanding and improvement strategies of interfacial Li+ transfer kinetics presented herein will be a foundation for designing high-rate lithium-ion batteries.

Keywords: activation energy; electrode/electrolyte interface; frequency factor; ion transfer; lithium-ion battery.