Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition

Abstract The growing demand for lithium batteries with higher energy densities requires new electrode chemistries. Lithium metal is a promising candidate as the anode material due to its high theoretical specific capacity, negative electrochemical potential and favorable density. However, during cycling, low and uneven lithium ion concentration on the surface of anode usually results in uncontrolled dendrite growth, especially at high current densities. Here we tackle this issue by using lithiophilic montmorillonite as an additive in the ether-based electrolyte to regulate the lithium ion concentration on the anode surface and thus facilitate the uniform lithium deposition. The lithiophilic montmorillonite demonstrates a pumping feature that improves the self-concentrating kinetics of the lithium ion and thus accelerates the lithium ion transfer at the deposition/electrolyte interface. The signal intensity of TFSI − shows negligible changes via in situ Raman tracking of the ion flux at the electrochemical interface, indicating homogeneous ion distribution, which can lead to a stable and uniform lithium deposition on the anode surface. Our study indicates that the interfacial engineering induced by the lithiophilic montmorillonite could be a promising strategy to optimize the lithium deposition for next-generation lithium metal batteries.