Introduction

All-solid-state batteries (ASSBs) have emerged as a promising alternative to conventional lithium-ion batteries, offering enhanced safety and the potential for higher energy densities. This mini-review focuses on recent advancements in ASSBs over the past five years, based on the provided papers. We will examine progress in three key areas: interface engineering, halide-based solid electrolytes, and composite polymer electrolytes.

Interface Engineering for Enhanced Stability and Performance

A significant challenge in ASSBs is the high interfacial resistance between the solid electrolyte and the electrodes, particularly the lithium metal anode. Researchers have focused on strategies to improve interfacial contact, stability, and ion transport.

Chunsheng Wang's research group at the University of Maryland has been actively involved in interface design. In 2023, they highlighted the importance of interface design for all-solid-state lithium batteries (Hongli Wan et al., 2023, Nature). More recently, in 2024, they explored the design of lithium anode interlayers for all-solid-state lithium-metal batteries (Zeyi Wang et al., 2024, Nature Energy) and investigated single-phase local-high-concentration solid polymer electrolytes for lithium-metal batteries (Weiran Zhang et al., 2024, Nature Energy). These studies emphasize the crucial role of interfacial modification in enabling stable lithium metal cycling.

Xin Li's group at Harvard University has also contributed to this area. They introduced a dynamic stability design strategy for lithium metal solid-state batteries in 2020 (Luhan Ye et al., 2020, Nature) and 2021 (Luhan Ye et al., 2021, Nature). In 2024, they demonstrated that fast cycling of lithium metal in solid-state batteries can be achieved by using constriction-susceptible anode materials (Luhan Ye et al., 2024, Nature Materials).

Yoon Seok Jung's research group at Korea Advanced Institute of Science and Technology (KAIST) has explored the use of protective layers. In 2024, they presented a rationally designed conversion-type lithium metal protective layer for all-solid-state lithium metal batteries (Haechannara Lim et al., 2024, Advanced Energy Materials).

Peter G. Bruce's group at the University of Oxford has focused on understanding dendrite formation and propagation. They visualized plating-induced cracking in lithium-anode solid-electrolyte cells in 2021 (Ziyang Ning et al., 2021, Nature Materials) and further investigated dendrite initiation and propagation in lithium metal solid-state batteries in 2022 (Ziyang Ning et al., 2022, Nature) and 2023 (Ziyang Ning et al., 2023, Nature).

Wei Luo's group at the University of Science and Technology of China (USTC) developed a self-regulated gradient interphase for dendrite-free solid-state Li batteries (Tengrui Wang et al., 2022, Energy & Environmental Science). They also explored promoting high-voltage stability through local lattice distortion of halide solid electrolytes (Zhenyou Song et al., 2024, Nature Communications).

These studies collectively demonstrate the importance of interface engineering in improving the performance and stability of ASSBs. Key strategies include the use of interlayers, protective coatings, and the design of electrolytes that promote uniform lithium deposition.

Advancements in Halide-Based Solid Electrolytes

Halide-based solid electrolytes have gained significant attention due to their high ionic conductivity and relatively low cost. Several research groups have focused on developing and optimizing these materials.

Xueliang Sun's group at the University of Western Ontario has made significant contributions to this area. They reviewed the prospects of halide-based all-solid-state batteries in 2022 (Changhong Wang et al., 2022, Science Advances) and explored structural regulation of halide superionic conductors for all-solid-state lithium batteries in 2024 (Xiaona Li et al., 2024, Nature Communications). They also developed a superionic amorphous NaTaCl6 halide electrolyte for highly reversible all-solid-state Na-ion batteries (Yang Hu et al., 2024, Matter). In 2020, they investigated site-occupation-tuned superionic Li_<i>x</i>ScCl_3+<i>x</i> halide solid electrolytes (Jianwen Liang et al., 2020, Journal of the American Chemical Society).

Yoon Seok Jung's group at KAIST has also been active in this field. They compared single- or poly-crystalline Ni-rich layered cathodes with sulfide or halide solid electrolytes in 2021 (Yoonjae Han et al., 2021, Advanced Energy Materials). They developed new cost-effective halide solid electrolytes in 2021 (Hiram Kwak et al., 2021, Advanced Energy Materials) and focused on boosting the interfacial superionic conduction of halide solid electrolytes in 2023 (Hiram Kwak et al., 2023, Nature Communications).

Yoshiaki Tanaka's group developed new oxyhalide solid electrolytes with high lithium ionic conductivity in 2022 (Yoshiaki Tanaka et al., 2022, Angewandte Chemie International Edition) and 2023 (Yoshiaki Tanaka et al., 2023, Angewandte Chemie International Edition).

Cheng Ma's group at the Chinese Academy of Sciences developed a cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte (Lv Hu et al., 2023, Nature Communications).

These studies highlight the ongoing efforts to develop and optimize halide-based solid electrolytes for ASSBs. The focus is on improving ionic conductivity, reducing cost, and enhancing interfacial compatibility with electrodes.

Composite Polymer Electrolytes for Enhanced Flexibility and Processability

Polymer electrolytes offer advantages such as flexibility, ease of processing, and good interfacial contact with electrodes. However, their ionic conductivity is generally lower than that of inorganic solid electrolytes. Researchers have explored the use of composite polymer electrolytes to enhance their performance.

Ce-Wen Nan's group at Tsinghua University has focused on tailoring inorganic-polymer composites for the mass production of solid-state batteries, publishing reviews in both 2020 (Li‐Zhen Fan et al., 2020, Nature Reviews Materials) and 2021 (Li‐Zhen Fan et al., 2021, Nature Reviews Materials).

Jinping Liu's group at the Beijing Institute of Technology has also contributed to this area. They designed a polymer-in-salt electrolyte and fully infiltrated 3D electrode for integrated solid-state lithium batteries in 2021 (Wenyi Liu et al., 2021, Angewandte Chemie International Edition) and developed a filler-integrated composite polymer electrolyte for solid-state lithium batteries in 2022 (Shuailei Liu et al., 2022, Advanced Materials).

Yi Cui's group at Stanford University developed scalable, ultrathin, and high-temperature-resistant solid polymer electrolytes for energy-dense lithium metal batteries (Yinxing Ma et al., 2022, Advanced Energy Materials).

Yunhui Huang's group at Huazhong University of Science and Technology (HUST) enabled all-solid-state Li metal batteries operated at 30 °C by molecular regulation of polymer electrolyte (Ying Wei et al., 2023, Advanced Energy Materials) and developed interfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries (Fei Pei et al., 2024, Nature Communications).

Xin Guo's group at Qingdao University of Science and Technology focused on tailoring polymer electrolyte ionic conductivity for production of low- temperature operating quasi-all-solid-state lithium metal batteries (Zhuo Li et al., 2023, Nature Communications).

These studies demonstrate the ongoing efforts to improve the performance of composite polymer electrolytes for ASSBs. Key strategies include the incorporation of inorganic fillers, the use of polymer-in-salt electrolytes, and the development of self-healing polymers.

Conclusion

The field of all-solid-state batteries has witnessed significant progress in the past five years. Research efforts have focused on interface engineering, the development of halide-based solid electrolytes, and the optimization of composite polymer electrolytes. These advancements have led to improved ionic conductivity, enhanced interfacial stability, and increased energy density. While challenges remain, the ongoing research and development in these areas are paving the way for the widespread adoption of ASSBs in the future.

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