Surface Functionalization of a Conventional Polypropylene Separator with an Aluminum Nitride Layer toward Ultrastable and High-Rate Lithium Metal Anodes

Lithium (Li) metal as a next-generation anode has received great interest from industry and academic institutes due to its attractive benefits of a high theoretical capacity (3860 mAh g(-1)) and the lowest negative potential (-3.04 V vs SHE) among the anode candidates. However, major issues associated with dendritic Li growth, infinite volume expansion of Li, and low Coulombic efficiency cause severely degraded cycle stabilities and fatal safety issues (such as short-circuit). Herein, we first designed a functional membrane, comprising an aluminum nitride (AlN) layer and a polypropylene (PP) separator, in order to curb the sharp Li dendrite growth, restrain the propagation of dendritic Li toward the PP separator, and consequently improve the electrochemical stabilities of Li metal batteries. When the designed membrane was introduced in either the Li/Cu half-cell or the Li/LCO full-cell, Li dendrite growth was significantly suppressed and side reactions associated with electrode degradation was effectively prevented by the material benefits of the AlN layer, thus leading to the significantly enhanced cycle performances. Low temperature stability tests further demonstrated the optimiztic potentiality of the designed membrane for enabling the stable operation of Li metal batteries under harsh conditions. Our approach of adopting a metal nitride layer to the PP separator can be a compelling strategy to improve the long-term electrochemical stability of the Li metal electrode.