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<p>Lithium argyrodites (e.g., Li<sub>6</sub>PS<sub>5</sub>X, X = Cl, Br, I) have emerged as highly promising solid electrolytes for all-solid-state lithium batteries (ASSLBs) owing to their exceptional ionic conductivity and favorable mechanical properties. However, their commercialization is severely hindered by the energy-intensive, complex, and poorly scalable nature of conventional solid-state synthesis. Recently, wet-chemical (liquid-phase) synthesis has attracted significant attention as a promising platform that can address several key limitations, offering not only molecular-level precursor mixing but also direct compatibility with slurry or infiltration-based electrode fabrication. This review provides a comprehensive overview of the latest advancements in the wet-chemical processing of Li-argyrodites. It systematically examines the critical role of solvent engineering, highlighting how the judicious selection of protic and aprotic solvents dictates precursor dissolution, reaction pathways, and the suppression of impurity phases. Furthermore, we discuss state-of-the-art kinetic and microstructural control strategies—such as microwave-assisted synthesis, cascade dissolution coprecipitation (CDC), and size-controlled wet-synthesis (SCWS)—which decouple rigid thermodynamic constraints to achieve uniform, highly conductive solid electrolytes. Crucially, we highlight how this reaction-controlled platform unlocks enhanced compositional expandability, enabling the low-temperature synthesis of halogen-rich phases, aliovalent dual-cation substituted frameworks, and thermally fragile cluster-anion incorporated superionic conductors. Finally, I outline the remaining challenges that must be addressed for practical ASSLB implementation, including scalable process validation, solvent recyclability and residual-solvent management, interfacial stabilization, and the fabrication of ultra-thin electrolyte membranes. By linking solvent-mediated reaction chemistry with electrode-level processability, this review highlights wet-chemical engineering as a key strategy for advancing high-energy-density ASSLBs.</p>

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Recent advances in wet-chemical processing of argyrodite-type sulfide solid electrolytes: reaction chemistry, solvent engineering, and scalable processing

  • 期刊论文

  • 发表日期：

    2026年8月3日

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  • Seung-Deok Seo

摘要

Lithium argyrodites (e.g., Li6PS5X, X = Cl, Br, I) have emerged as highly promising solid electrolytes for all-solid-state lithium batteries (ASSLBs) owing to their exceptional ionic conductivity and favorable mechanical properties. However, their commercialization is severely hindered by the energy-intensive, complex, and poorly scalable nature of conventional solid-state synthesis. Recently, wet-chemical (liquid-phase) synthesis has attracted significant attention as a promising platform that can address several key limitations, offering not only molecular-level precursor mixing but also direct compatibility with slurry or infiltration-based electrode fabrication. This review provides a comprehensive overview of the latest advancements in the wet-chemical processing of Li-argyrodites. It systematically examines the critical role of solvent engineering, highlighting how the judicious selection of protic and aprotic solvents dictates precursor dissolution, reaction pathways, and the suppression of impurity phases. Furthermore, we discuss state-of-the-art kinetic and microstructural control strategies—such as microwave-assisted synthesis, cascade dissolution coprecipitation (CDC), and size-controlled wet-synthesis (SCWS)—which decouple rigid thermodynamic constraints to achieve uniform, highly conductive solid electrolytes. Crucially, we highlight how this reaction-controlled platform unlocks enhanced compositional expandability, enabling the low-temperature synthesis of halogen-rich phases, aliovalent dual-cation substituted frameworks, and thermally fragile cluster-anion incorporated superionic conductors. Finally, I outline the remaining challenges that must be addressed for practical ASSLB implementation, including scalable process validation, solvent recyclability and residual-solvent management, interfacial stabilization, and the fabrication of ultra-thin electrolyte membranes. By linking solvent-mediated reaction chemistry with electrode-level processability, this review highlights wet-chemical engineering as a key strategy for advancing high-energy-density ASSLBs.