Elastic and Li-ion–percolating hybrid membrane stabilizes Li metal plating

Significance Lithium metal batteries are capable of revolutionizing the battery marketplace for electrical vehicles. They are, however, plagued by the reactive Li metal–electrolyte interface and growth of Li dendrites on cycling, which pose concerns to both cell performance and safety. We demonstrate that a Li metal negative electrode can be stabilized by a hybrid inorganic/organic membrane that is grown directly onto it. A solid electrolyte phase offers percolated Li + -ion–conducting channels and the infiltration of an elastic polymer endows membrane flexibility to accommodate volume changes. The protected electrode allows Li deposition/stripping with 95.8% efficiency and stable operation of an electrochemical cell for 2,000 cycles. This rationally structured membrane represents an interface engineering approach toward stabilized Li metal electrodes.