Investigation of Electron Spin Polarization-Regulated Lithium Metal Deposition Behavior and Its Interfacial Mechanisms

Abstract

Abstract: Lithium metal anodes, featuring an ultrahigh theoretical specific capacity and a low electrochemical potential, are widely regarded as promising candidates for next-generation high-energy-density batteries. However, their practical implementation remains hindered by interfacial instability, dendritic lithium growth, and limited reversibility of lithium plating/stripping. ESP provides an emerging electronic-structure perspective for understanding interfacial electron transfer and regulating interfacial reactions during lithium deposition. This review focuses on magnetism-related strategies, including spin-polarized interfaces, magnetic hosts, and external magnetic fields, and systematically delineates the mechanistic distinctions among ESP regulation, magnetic-response effects, and magnetohydrodynamic effects. In particular, the potential roles of spin-resolved electronic structures in interfacial charge redistribution, Li⁺/electron coupling, and uniform lithium deposition are summarized, with the aim of providing theoretical guidance for the rational design of highly stable lithium metal anodes.