Abstract

Li metal is the ultimate anode material for Li based battery with high energy density. However, inhomogeneous charge distribution from the unbalanced ion/electron transport is usually generated at the electrode surface, leading to the uncontrollable dendrites with poor reversibility. Herein, interconnected Li 3 P@Cu ion/electron conductive interlayer activated from interfacial reaction between Cu 3 P arrays and metallic Li is efficiently constructed on Li foil surface through room-temperature mechanical rolling process for charge redistribution. Demonstrated by theoretic calculation, the diffusion barrier of Li + is remarkably reduced from Li 3 P interphase with high ionic conductivity, while the electron-conductive Cu domains ensures well-dispersed current density, facilitating the uniform distribution of interfacial Li + flux. Furthermore, the interconnected skeletons with extensive active channels significantly enhances the electrochemical kinetics and promotes the reversibility of Li plating/stripping processes. As expected, a prolonged lifespan of symmetrical cells over 1500 h with lower polarization is successfully achieved at 1 mA cm −2 , further improving the rates and cycling performances of LiFePO 4 based full cells in mass loading of 8.5 mg cm −2 with a capacity retention up to 91.7% after 300 cycles. This work proposed a rational interlayer design for interfacial charge redistribution and presents an efficient strategy to realize dendrite-free Li metal anode. The practical application of Li metal battery is predominately retarded by the uncontrollable dendrite growth from unbalanced ion/electron transport. In this work, a room-temperature interfacial reaction was applied to construct Li 3 P/Cu mixed conductive layer for interfacial charge redistribution via a facial mechanical rolling press method. Interestingly, the derived coating layer with mixed ion/electron conductive feature significantly enhances the electrochemical kinetics and promotes the interfacial charge redistribution with a dendrite-free deposition morphology. Greatly, Li@MCI based symmetric cells achieves a prolonged lifespan over 1500 h at 1 mA cm −2 with lower polarization than that of Li based cells, which further promotes the rate performance and stability of the Li@MCI based full batteries with a high-loading LiFePO 4 cathode (8.5 mg cm −2 ). • Interconnected Li 3 P@Cu MCI was efficiently constructed on Li foil surface for interfacial charge redistribution. • Enhanced electrochemical Kinetics has been demonstrated by DFT calculations and symmetric cell. • Epitaxially growth of lithium was achieved within Li 3 P@Cu interlayer. • Li 3 P@Cu modified Li metal exhibited robust electrochemical performance over 1500 h.

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