The solid-state lithium metal batteries (SSLMBs) are considered to be promising next-generation batteries because of their high energy density and safety levels. The practical application of the SSLMBs is influenced by the solid polymer electrolytes (SPEs), which are a critical component of the SSLMBs; hence, the structural design of SPEs has always been extensively studied. Herein, the characteristics of polyether with ether groups and polycarbonate with carbonate groups as well as their development will be systematically discussed with respect to the functional groups; additionally, the synergistic effect of two functional groups in a copolymer and promising research directions to design SPEs exhibiting comprehensive performances are investigated. Subsequently, as the key factors affecting the development of SSLMBs with SPEs, the progress of lithium salts and achievements in interfacial modification will be discussed. Finally, the current condition of SSLMBs will be revealed. In addition, future perspectives will be provided to guide the future designs of polymer electrolytes for high-performance SSLMBs.

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Solid sulfide electrolyte has been researched for several years, and a high ionic conductivity has been acquired. However, it is difficult to apply in industrial manufacturing partly because the raw materials, such as SiS 2 , GeS 2 , P 2 S 5 , et al., have strict preparing conditions and are sensitive to water and oxygen in the air. Herein, we report a new method to produce solid sulfide electrolytes Li 9.54 Si 1.74 P 1.44 S 11.7 X 0.3 (LSiPSX) (X = F, Cl, Br, I), that is, using elementary substances Si, P, and S as the starting raw materials, which not only is a promising way to ease the harsh storage conditions of the SiS 2 and P 2 S 5 as starting raw materials but also provides a feasible choice for the preparation of solid sulfide electrolyte. The conductivity of solid sulfide electrolyte is further adjusted by controlling the particle size of raw material silicon and the different halogen doping. As a result, the Li 9.54 Si 1.74 P 1.44 S 11.7 I 0.3 releases the highest ionic conductivity of 1.35 mS/cm at room temperature and a wide electrochemical window up to 9 V versus Li/Li + which is prepared from the 3 nm particle size Si and I doping. The all-solid-state lithium−sulfur battery (ASSLSB) is constructed with LSiPSI and with a good performance. Our study demonstrates the possibility of preparing the LGPS crystal type solid sulfide electrolytes by using elementary substances.