Understanding the Effects of Interfacial Lithium Ion Concentration on Lithium Metal Anode

Despite the development of multidimensional state‐of‐the‐art electrode materials for constructing better lithium metal anodes (LMAs), the key factors influencing the electrochemical performance of LMAs are still poorly understood. Herein, it is demonstrated that the local lithium ion concentration at the interface between the electrode and electrolyte exerts significant influence on the electrochemical performance of LMAs. The local ion concentration is multiplied by introducing pseudocapacitive nanocarbons (PNCs) containing numerous heteroatoms, because PNCs can store large numbers of lithium ions in a pseudocapacitive manner, and promote the formation of an electrochemical double layer. The high interfacial lithium ion concentration induces the formation of lithium‐rich inorganic solid–electrolyte–interface layers with high ionic conductivities, and facilitates sustainable and stable supplies of lithium ion charge carriers on the overall active surfaces of the PNCs. Accordingly, the PNC‐induced LMA exhibits high Coulombic efficiencies, high rate capabilities, and stable cycling performance.