A strongly interactive adatom/substrate interface for dendrite-free and high-rate Li metal anodes

Abstract

Lithium (Li) metal is considered as one of the most promising anode materials to build next-generation high-energy–density batteries. Nonetheless, dendritic Li deposition has dramatically hindered the practical applications of Li metal batteries (LMBs). Uniformizing Li deposition is a prerequisite to achieve safe and practical LMBs. Herein, an underpotential deposition (UPD) process is first proposed to alter the kinetic and uniformity of Li deposition morphology. Based on the strong interaction between the Li adatoms and manganese (Mn) based substrate, a competition between the UPD and bulk Li deposition is observed, on which the predominance of the UPD scenario tends to uniformize Li nucleation and deposition by the surface coverage of Li monolayers at potentials that are more positive than the Nernst potential of Li metal. Inspired by this process, an advanced hybrid Mn-graphene oxide structure is developed for Li protection, not only enabling dendrite-free Li anodes for high-capacity and -current density cycling, but also improving the interfacial kinetic of Li metal anodes at subzero temperatures, showing potential applicability in low temperature conditions.