Harnessing Database-Supported High-Throughput Screening for the Design of Stable Interlayers in Halide-Based All-Solid-State Batteries

All-solid-state Li metal batteries (ASSLMBs) promise superior safety and energy density compared to conventional Li-ion batteries. However, their widespread adoption is hindered by detrimental interfacial reactions between solid-state electrolytes (SSEs) and the Li anode, compromising long-term cycling stability. The challenges in directly observing these interface layers have impeded a comprehensive understanding of reaction mechanisms, necessitating first-principle simulations for the design of novel interlayer materials. To address these challenges, we developed a database-supported high-throughput screening (DSHTS) framework for identifying stable interlayer materials compatible with both Li and SSEs. Using Li₃InCl₆ as a model SSE, we identified Li₃OCl as a promising interlayer material. Experimental validation demonstrated excellent electrochemical performance in both symmetric- and full-cell configurations. A Li|Li₃OCl|Li₃InCl₆|LiCoO₂ cell exhibited an initial discharge capacity of 154.4 mAh g⁻¹ at 1C with 76.36% capacity retention after 1000 cycles. In contrast, a cell with a traditional In-Li₆PS₅Cl interlayer delivered only 132.4 mAh g⁻¹ at 1C and failed after 760 cycles. An additional interlayer-containing battery with Li(Ni_0.8Co_0.1Mn_0.1)O₂ as the positive electrode achieved an initial discharge capacity of 151.3 mAh g⁻¹ at 3C, maintaining stability over 1650 cycles. The results demonstrate the promise of the DSHTS framework for identifying interlayer materials. Our approach opens new avenues for SSE-based battery development, paving the way for next-generation ASSLMB with significantly enhanced stability.