Li^(+)Solvation Mediated Interfacial Kinetic of Alloying Matrix for Stable Li Anodes

Severe lithium(Li)dendrite growth caused by the uneven overpotential deposition is a formidable challenge for high energy density Li metal batteries(LMBs).Herein,we investigate a synergetic interfacial kinetic to regulate Li deposition behavior and stabilize Li metal anode.Through constructing Li alloying matrix with a bi-functional silver(Ag)-Li_(3)N blended interface,fast Li^(+)conductivity and high Li affinity can be achieved simultaneously,resulting in both decreased Li nucleation and mass transfercontrolled overpotentials.Beyond these properties,a more important feature is demonstrated herein;that is,the inward diffusion depth of the Li adatoms inside of the Ag site can be restricted by the Li^(+)solvation structure in a highly coordinating environment.The latter feature can ensure the durability of the operational Ag sites,thereby elongating the Li protection ability of the Ag-Li_(3)N interface greatly.This work provides a deep insight into the synergetic effect of functional alloying structure and Li^(+)solvation mediated interfacial kinetic on Li metal protection.

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

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.