Negatively Charged Holey Titania Nanosheets Added Electrolyte to Realize Dendrite‐Free Lithium Metal Battery

Abstract Electrolyte modulation and electrode structure design are two common strategies to suppress dendrites growth on Li metal anode. In this work, a self‐adaptive electrode construction method to suppress Li dendrites growth is reported, which merges the merits of electrolyte modulation and electrode structure design strategies. In detail, negatively charged titania nanosheets with densely packed nanopores on them are prepared. These holey nanosheets in the electrolyte move spontaneously onto the anode under electrical field, building a mesoporous structure on the electrode surface. The as‐formed porous electrode has large surface area with good lithiophilicity, which can efficiently transfer lithium ion (Li + ) inside the electrode, and induce the genuine lithium plating/stripping. Moreover, the negative charges and nanopores on the sheets can also regulate the lithium‐ion flux to promote uniform deposition of Li metal. As a result, the symmetric and full cells using the holey titania nanosheets containing electrolyte, show much better performance than the ones using electrolyte without holey nanosheets inside. This work points out a new route for the practical applications of Li‐metal batteries.