Abstract The low coulombic efficiency and poor cycle performance deriving from uncontrolled growth of dendrites have caused a serious obstacle to the practical application of lithium metal. Herein we propose… Click to show full abstract
Abstract The low coulombic efficiency and poor cycle performance deriving from uncontrolled growth of dendrites have caused a serious obstacle to the practical application of lithium metal. Herein we propose a bifunctional regular-random dual cross-linking network solid polymer electrolyte (RRa-SPE) for dendrite-free all-solid-state lithium metal batteries. Under the synergistic effect of regular polymerization skeleton and random cross-linking network, the RRa-SPE effectively regulates the lithium deposition and facilitates the generation of a highly homogeneous and robust solid-electrolyte interphase (SEI) layer on lithium metal. Besides, this RRa-SPE shows benign ionic conductivity of 4.36 × 10−4 S cm−1 (at 30 °C), high lithium ion transference number of 0.76 and enhanced mechanical strength. The Li/RRa-SPE/Li symmetric cell maintains low and stable voltage polarization (0.15 V) after circulating for 1200 h at 0.5 mA cm−2. Improved LiFePO4/RRa-SPE/Li cell exhibits excellent rate capability and prominent cycle performance with a capacity retention of 99.6% after 240 cycles at 0.5 C at 30 °C.
               
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