Lithiophilic Interphase Porous Buffer Layer toward Uniform Nucleation in Lithium Metal Anodes

Abstract Lithium metal batteries are highly desired for durable and high‐power energy storage devices due to high theoretical capacity and lowest redox potential. Nevertheless, high activity of Li, large volume change, and Li dendrite formation during cycling severely hinder their further application. Herein, an inventive Cu collector decorated with holey MoO 2 ‐Mo 3 N 2 heterojunction nanobelts‐coated reductive graphene oxide (G‐MoO 2 ‐Mo 3 N 2 , GMM) for high‐performance Li metal batteries is reported. The collector features synergistic functions of remarkable lithiophilicity, a built‐in electric field formed by splendid interfacial contact, and dense lithiophilic‐enriched solid electrolyte interphase layer. They facilitate robust charge transfer and ionic diffusion, and meliorate inhomogenous Li‐ion flux for inhibiting the growth of dendrites. In addition, the incorporation of flexible graphene layer enhances the structural integrity and electron transport kinetics. Remarkably, it is demonstrated that GMM significantly enhances Coulombic efficiency of ≈99.5% over 1566 cycles (0.5 mA cm −2 /0.5 mAh cm −2 ). Furthermore, excellent cycling and rate capability of full cells with the GMM@Cu anode and high areal loading of LiFePO 4 cathode (22.2 mg cm −2 ) are also realized. This work illustrates the superiority of synergetic design of lithiophilic sites plus electron transport kinetics for the current collector of Li‐metal anode to seek the high energy density.