Tailoring the Mechanical and Electrochemical Properties of an Artificial Interphase for High‐Performance Metallic Lithium Anode

Lithium metal is regarded as the “Holy Grail” of anode materials due to its low electrochemical potential and high theoretical capacity. Unfortunately, its unstable solid electrolyte interphase (SEI) leads to low Coulombic efficiency (CE) and serious safety issues. Herein, a hybrid nanoscale polymeric protective film with tunable composition and improved stiffness is developed by incorporating aluminum crosslinkers into the polymer chains. The Li plating/stripping process is regulated through the protective coating and the dendrite growth is effectively suppressed. Promisingly, the protected Li can deliver stable performance for more than 350 h with a cycling capacity of 2 mAh cm−2 without a notable increase in overpotential. Moreover, a stable charge/discharge cycling in Li–O2 batteries with the protected Li can be maintained for more than 600 h. This work provides guidance on the rational design of electrode interfaces and opens up new opportunities for the fabrication of next‐generation energy storage systems. Polyurea with aluminum crosslinkers is deposited on a Li metal anode to serve as a robust nanoscale artificial solid‐electrolyte interphase. The stiffness of the polyurea thin film is improved significantly due to the addition of an inorganic crosslinker. The protected Li metal anode enables a stable long cycling life for a Li–O2 battery for more than 600 h.