Multiscale interfacial engineering strategies for inorganic all-solid-state lithium batteries

Abstract

All-solid-state lithium batteries (ASSLBs) offer exceptional energy density and safety, yet interfacial instability at both cathode and anode remains a major challenge. This review pioneers a unified, multiscale framework that systematically dissects interfacial failure mechanisms across mainstream inorganic solid-state electrolytes (SSEs)—including oxides, sulfides, and halides—under multiphysics coupling. Unlike previous studies focusing on isolated materials or single strategies, we provide a critical, side-by-side comparison of leading interface engineering routes—electrode engineering, interlayer construction, electrolyte regulation, and integrated dual-interface design—emphasizing their respective merits, limitations, and application boundaries. Furthermore, advanced characterization techniques are summarized to reveal dynamic interfacial evolution and validate the effectiveness of various engineering approaches, thereby bridging fundamental understanding with practical design. Finally, future perspectives highlight multiphysics characterization, machine-learning-assisted interface material screening, and scalable process integration. This review offers a comprehensive, comparative, and practical guide to interface innovation in high-performance ASSLBs.