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Highlights: The lithium-ion conduction mechanism of organic-inorganic composite solid electrolytes (OICSEs) is thoroughly conducted and concluded from the microscopic perspective based on filler content, type, and system. The classic inorganic filler types, including inert and active fillers, are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of OICSEs. Advanced characterization techniques for OICSEs are discussed, and the challenges and prospects for developing superior all-solid-state lithium batteries are highlighted. To address the limitations of contemporary lithium-ion batteries, particularly their low energy density and safety concerns, all-solid-state lithium batteries equipped with solid-state electrolytes have been identified as an up-and-coming alternative. Among the various SEs, organic–inorganic composite solid electrolytes (OICSEs) that combine the advantages of both polymer and inorganic materials demonstrate promising potential for large-scale applications. However, OICSEs still face many challenges in practical applications, such as low ionic conductivity and poor interfacial stability, which severely limit their applications. This review provides a comprehensive overview of recent research advancements in OICSEs. Specifically, the influence of inorganic fillers on the main functional parameters of OICSEs, including ionic conductivity, Li+ transfer number, mechanical strength, electrochemical stability, electronic conductivity, and thermal stability are systematically discussed. The lithium-ion conduction mechanism of OICSE is thoroughly analyzed and concluded from the microscopic perspective. Besides, the classic inorganic filler types, including both inert and active fillers, are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of OICSEs. Finally, the advanced characterization techniques relevant to OICSEs are summarized, and the challenges and perspectives on the future development of OICSEs are also highlighted for constructing superior ASSLBs. [ABSTRACT FROM AUTHOR]

Solid-state electrolytes with high room temperature ionic conductivity, broad electrochemical window, and favorable thermal stability are crucial for the practical application of all-solid-state lithium-metal batteries. Here, a novel succinonitrile (SN)-based composite solid-state electrolyte (SN-CSSE) is fabricated directly inside the glass-fiber (GF) membrane via in-situ thermal-crosslinking ethoxylate trimethylolpropane triacrylate (ETPTA) monomer, coupled with the liquid SN-based electrolyte. The ionic conductivity, oxidation potential and lithium-ion transference number (T Li +) of SN-CSSE are 0.78 mS/cm, 5.20 V (vs. Li/Li+) and 0.68 at ambient temperature, respectively. The coin full cells equipped with high-voltage LiCoO 2 (LCO) and modified Li metal anode deliver excellent interfacial stability, cycling reversibility, and rate capability. Moreover, the LCO/SN-CSSE/Li pouch cell exhibits more superior thermal stability than that of cell with commercial carbonate-based electrolyte during thermal shock test. • SN-CSSE formed by in-situ thermal polymerization technology. • SN-CSSE with high ionic conductivity, oxidative resistance, and T Li +. • LCO/SN-CSSE/T-Li coin cell displays high electrochemical performances. • LCO/SN-CSSE/T-Li pouch cell shows high thermal stability. [ABSTRACT FROM AUTHOR]

• The real electrochemical stability of organic-inorganic CSSE is confirmed by simulating the real working environment. • Capacity fading mechanisms of 4 V-class ASSLPBs are elucidated by systematic electrochemical testing and physical characterization. • Two targeted modification methods for 4 V-class ASSLPBs are proposed. Owing to high safety and considerable energy density, rechargeable all-solid-state lithium-metal polymer batteries (ASSLPBs) with organic-inorganic composite solid-state electrolytes (CSSEs) have been recognized as one of the most promising battery systems. However, 4 V or above-class ASSLPBs still suffer serious capacity degradation arising from the complex interface issues between the electrode and electrolyte. Herein, for the first time, we find the oxidation decomposition of TFSI- anion and further interaction with PEO polymer matrix in the LiNi 0.8 Co 0.1 Mn 0.1 LiO 2 (NCM811)/CSSEs (PEO-LiTFSI-LAGP)/Li cell, which cause continuous damage to the interfacial stability and persistent capacity degradation. Increasing the ratio of LAGP filler in CSSEs membrane and employing PEO-LiBOB electrolyte in composite cathode were demonstrated effective. As a consequence, the ASSLPBs show high reversibility, and high capacity retention up to 88% (3.0–4.2 V) and 78% (3.0–4.3 V) after 100 cycles with the charge/discharge current density of 30 mA g−1 (35 °C). The understanding on capacity degradation mechanism, along with the positive improvement strategies validly boosts the development and promising application of 4 V-class ASSLPBs. [ABSTRACT FROM AUTHOR]