Hybrid solid electrolyte (HSE) exhibits potential as a solid electrolyte due to its satisfactory Li+ conductivity, superior flexibility, and optimal interface compatibility. However, the inadequate wettability of the Li/HSE interface leads to significant contact impedance, thus fostering the formation of Li dendrites and limiting their practical applicability. Here, a straightforward strategy to enhance the interfacial wettability between Li and HSE and promote the uniform migration of Li+ by in situ construction of a multifunctional interface consisting of Li3P/LiCl (PCl@Li) was created. The Li3P component acts as a Li+ channel, banishing Li+ diffusion obstacles within the interface layer, while the electronically insulating LiCl component acts as an electron-blocking shield at the Li/HSE interface, promoting uniform Li+ deposition and preventing the formation of Li dendrites. The interface impedance of the symmetric PCl@Li|HSE|PCl@Li battery decreases markedly from 230.2 to 47.4 Ω cm–2. Additionally, the battery demonstrates superb cycling stability for over 1300 h at 0.1 mA cm–2 and maintains a minimal overpotential of 32 mV at 30 °C. The PCl@Li|HSE|LiFePO4 battery shows an initial discharge-specific capacity of 135.6 mA h g–1 at 1 C, with a notable capacity retention of 87.0% (118.0 mA h g–1) after 500 cycles. This work provides a new facile strategy for all-solid-state batteries to address interface issues between Li electrodes and HSE.
Li metal anodes as one of promising anodes in next-generation batteries , face the challenges from infinite volume change and high reactivity to electrolytes that easily leads to unstable Li/electrolyte interface and unique dendrite growth of Li. Although mechanical pressure can effectively inhibit the dendrite growth of Li, it also increases the risk of short circuits, because Li metal easily grows into the separator under pressure. Here, an interface layer is introduced on Li metal to block this growth, using Li 3 P/LiCl as a model. Meanwhile, the dense and robust layer also reduce the side reactions between Li and electrolytes. With the helps from mechanical pressure and interface layer , this design exhibits the improved electrochemical performances, much better than that without pressure or without the layer. The full cells of Li 3 P/LiCl-coated Li//LiFePO 4 , show a capacity of 1.69 mAh cm −2 after 1000 cycles under pressure at 3.9 mA cm −2 with a capacity retention of 99.5% in carbonates. The results indicate the promising potential for the pressure effect to be used for advanced Li metal anodes .
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