Insight into the Interface Design for Li Metal Anode: Organic‐Rich or Inorganic‐Rich

Abstract Microcracks and surface heterogeneity in solid‐electrolyte interphase (SEI) induced by repeated plating/stripping of lithium (Li) metal exacerbate SEI fracture propagation and dendrite growth, which lead to unsatisfactory Coulombic efficiency and limited cycle life of Li metal anode. In this study, the hybrid artificial interfaces with controlled organic–inorganic ratios are designed and deep insight into their impacts on the electro‐chemo‐mechanical properties is obtained. The organic–inorganic ratios in the hybrid interfaces influence the mechanical properties, lithiophilicity, and diffusion kinetics of the interfaces, which in turn affect the nucleation, early growth, and repeated deposition/dissolution behavior of Li. It is found that increasing the inorganic ratio in the hybrid interface can realize significantly enhanced electrochemical performances. This work answers a key question for hybrid interfaces: should organic‐rich or inorganic‐rich be preferred in the hybrid interface? It is believed that this work will guide the future design of hybrid interfaces for Li metal anode and open up opportunities for the realization of next‐generation Li metal batteries.