Darzin International Company Multidisciplinary Engineering Science Open 1 Serial Number 1 2024 02 01 Solid-State Electrolytes: Structure–Ionics–Interface Coupling in Next-Generation Batteries Solid-State Electrolytes: Structure–Ionics–Interface Coupling in Next-Generation Batteries 1 11 EN Journal Article 2023 11 24 <p>This study aims to synthesize current knowledge on solid-state electrolytes by examining the interdependent relationships among structural architecture, ionic transport, and interface coupling to inform the design of next-generation all-solid-state batteries. A qualitative systematic review was conducted using 25 high-impact peer-reviewed articles published between 2018 and 2025, focusing on ceramic, sulfide, halide, and composite solid-state electrolytes. Data were collected exclusively via literature review and analyzed using NVivo 14 software to perform open, axial, and selective coding, achieving theoretical saturation. Key variables extracted included crystal structure, defect chemistry, ionic conductivity, microstructure, electrode compatibility, interfacial stability, and mechanical robustness. Thematic analysis identified four overarching categories with multiple subthemes, encompassing structure, ionics, interface, and design integration. The review revealed that crystal structure and defect engineering directly influence ionic conductivity, with high-symmetry lattices and controlled vacancy distributions enhancing Li⁺ or Na⁺ mobility. Microstructural and composite design strategies, including grain refinement and polymer–ceramic hybrids, improve mechanical stability while facilitating continuous ion transport pathways. Interfacial coupling between electrolytes and electrodes was found to be critical for minimizing impedance and preventing degradation, with buffer layers, surface coatings, and stack pressure demonstrating efficacy in maintaining stable contact. The integration of structural, ionic, and interfacial considerations emerged as a holistic design principle, emphasizing that performance improvements depend on concurrent optimization across these dimensions. Emerging computational modeling and in-situ characterization techniques support predictive design and real-time monitoring of structure–ionics–interface interactions. Optimizing solid-state electrolytes requires a coupled approach that integrates atomic-scale structure, ion transport behavior, and interface engineering. Holistic design strategies, informed by multi-scale modeling, advanced characterization, and hybrid composite systems, are essential to advancing the commercial viability of all-solid-state batteries with high energy density, safety, and cycle life.</p> https://jmesopen.com/index.php/jmesopen/article/download/28/23