Lithiophilic Protective Dual Layer Enabling Stable Electrodeposition of Lithium at High Current Density

Abstract

Lithium (Li) is an ideal anode material for rechargeable batteries and thus manufacturing Li metal is crucial for the practical development of Li metal batteries. Electrodeposition is an efficient technique for producing ultrathin and scalable Li metal electrodes. However, the dendritic growth and the side reactions of Li with electrolyte during the electrodeposition are the main obstacles to overcome. In this study, we designed a pre-coated protective dual layer (PDL) composed of a poly(ethylene oxide)-based solid polymer electrolyte (SPE) and a polydopamine-coated cellulose membrane (PD-CM). The adhesive and ion-conductive SPE layer suppressed the growth of Li dendrites and side reactions with liquid electrolyte. The PD-CM layer with high porosity and lithiophilicity promoted a facile and uniform Li-ion flux. By applying the pre-coated PDL, Li was uniformly electrodeposited on the Ag-coated Cu at a high current density of 6 mA cm−2. The Li/LiFePO4 cell composed of an electrodeposited Li anode with PDL and a LiFePO4 cathode was assembled without an additional separator, and its cycling performance was evaluated. The cell initially delivered a high discharge capacity of 154.8 mAh g−1 at 45 °C and exhibited excellent cycling stability with a capacity retention of 97.0% after 200 cycles.