All-solid-state lithium-sulfur batteries (ASSLSBs) offer a means to enhance the energy density and safety of the state-of-art lithiumion batteries (LIBs), due to their high gravimetric energy density, low cost and environmental benignancy. In this work, the status of the research advances and perspectives on several types of solid electrolytes (SEs) developed for ASSLSBs are reviewed. The promises and challenges of utilizing SEs are discussed taking into account both theoretical calculation and experimental results, in hope of shedding some lights on future design of high energy density, cost competitive, and safe Li-S batteries. Lithium-sulfur (Li-S) batteries have been extensively investigated for lightweight applications (e.g., aircraft, artificial satellite, and unmanned aerial vehicles), and large-scale stationary energy storage, owing to their high gravimetric energy density, low cost, and environmental friendliness.1-3 The deployment of Li-S batteries into commercial market is hampered by several seemingly intrinsic problems resulting from the complex cell chemistry. Firstly, the electronically insulating nature of elemental sulfur (S 8 ) and end-product lithium sulfide (Li 2 S) leads to unstable electrochemical contact within S cathode. [4][5][6][7] Secondly, the soluble intermediates of polysulfide (PS) can diffuse between the cathode and anode (i.e., shuttle effect of PS), generating an active material loss in S cathode and degrading metallic Li anode. [4][5][6][7][8][9] Thirdly, the formation of 'dead' Li and Li dendrites upon cycling could not only decrease the Coulombic efficiency but also raise safety issues. [10][11][12] In recent years, various strategies have been attempted to overcome the above-mentioned problems. Most of the efforts have been devoted to enhance the electrochemical performance of Li-S batteries using well-designed cathode materials. 13 The diffusion of polysulfide species generated during discharge into electrolytes can be significantly suppressed by infusing sulfur into carbon materials in the cathode with an adequately controlled and engineered porosity and pore size, thus increasing the practical capacity and cyclability of Li-S batteries. These rational and creative strategies of cathode design have been covered by a number of recent reviews. 7,14,15 Besides, new binders (e.g., poly(ethylene oxide) (PEO) 16 and carboxymethycellulose (CMC) 17,18 ) have been employed for guarantying the integrity of the morphology and structure of S cathode, and enhancing the adhesion to current collector. The modification of separators (e.g., multiwall carbon nanotubes coated polypropylene 19 and lithiated Nafion 20 ) have been also developed for reducing the migration of polysulfides, thus mitigating the shuttle effect of PS.
21Apart from the strategies mentioned above, another approach, focusing on electrolyte formulation and modification, has been proved to be effective. The performances of Li-S batteries are largely affected by the electrolyte recipes, such as the type and identity of so...