All-solid-state lithium batteries (ASSLBs) are increasingly regarded as one of the next-generation energy storage technologies, offering good abuse tolerance, a wide operating temperature range, and a simplified battery system suitable for automotive applications. In the pursuit of cost-effectiveness and battery thermal stability, LiFePO4 (LFP) has recently attracted widespread attention in both industry and academia as a cathode active material for ASSLBs. However, the poor interfacial compatibility between the electrode and electrolytes has significantly hindered the development of LFP-based ASSLBs. In this study, an advanced Li2ZrCl6 (LZC) – Li9.54Si1.74P1.4S11.7Cl0.3 (LiSiPSCl) bilayer electrolyte is rationally designed for LFP-based ASSLBs, aiming to simultaneously achieve favorable interfacial compatibilities with both the LFP cathode layer and alloy anode layer. As a result, the developed LFP-LZC/LZC/LiSiPSCl/Li–In ASSLB can not only deliver a high initial discharge capacity of 144.9 mA h g−1, but also manifest a high-capacity retention up to 89% after 400 cycles at the current density of 1C. The strategy used in this work sheds light on a promising method to engineer stabilized interfaces for LFP-based ASSLBs.
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