(Digital Presentation) All-Solid-State Lithium Batteries: From Materials and Interface Design to Practical Pouch Cell Engineering

All-solid-state lithium batteries (ASSLBs) have gained substantial attention because of their intrinsic safety and high energy density. 1 However, the commercialization of ASSLBs has been stymied by insufficient ionic conductivity of solid-state electrolytes, significant interfacial challenges, as well as the large gap between fundamental research and practical engineering. Over the past several years, we have been dedicated to developing ASSLBs from solid electrolyte synthesis to interface design to engineering practical solid-state pouch cells. First , a wet-chemistry method with a low cost was proposed to produce solid-state electrolytes at the kilogram level with a high room-temperature ionic conductivity (> 1 mS.cm -1 ). 2 Second , the interfacial challenges of ASSLBs have been well addressed via increasing the ionic conductivity of interfacial buffer layers, 3 manipulating interfacial nanostructures, 4, 5 using single-crystal cathodes, 6 deciphering interfacial reaction mechanisms, 7 and constructing artificial solid electrolyte interphases (SEI), 8 which successfully boosted interfacial ion and electron transport kinetics. 9 Resultantly, ASSLBs demonstrated superior electrochemical performance. Third , practical solid-state pouch cells with high energy density have been engineered. Recently, a solvent-free process was proposed to fabricate freestanding and ultrathin inorganic solid electrolyte membranes. 10 Furthermore, a feasible solid-liquid transformable interface was devised to improve the solid-solid ionic contact and accommodate the significant volume change of solid-state pouch cells. 11, 12 The resultant solid-state pouch cells successfully demonstrated high energy density and unparalleled safety. In summary , our research not only provides an in-depth understanding of solid electrolyte synthesis and rational interface design but also offers feasible strategies to commercialize ASSLBs with high energy density, low cost, and excellent safety. References C. Wang, J. Liang, Y. Zhao, M. Zheng, X. Li and X. Sun, Energy Environ. Sci. , 2021, 14 , 2577-2619. C. Wang, J. Liang, J. Luo, J. Liu, X. Li, F. Zhao, R. Li, H. Huang, S. Zhao, L. Zhang, J. Wang and X. Sun, Sci. Adv. , 2021, 7 , eabh1896. C. Wang, J. Liang, S. Hwang, X. Li, Y. Zhao, K. Adair, C. Zhao, X. Li, S. Deng, X. Lin, X. Yang, R. Li, H. Huang, L. Zhang, S. Lu, D. Su and X. Sun, Nano Energy , 2020, 72 , 104686. C. Wang, X. Li, Y. Zhao, M. N. Banis, J. Liang, X. Li, Y. Sun, K. R. Adair, Q. Sun, Y. Liu, F. Zhao, S. Deng, X. Lin, R. Li, Y. Hu, T.-K. Sham, H. Huang, L. Zhang, R. Yang, S. Lu and X. Sun, Small Methods , 2019, 3 , 1900261. C. Wang, J. Liang, M. Jiang, X. Li, S. Mukherjee, K. Adair, M. Zheng, Y. Zhao, F. Zhao, S. Zhang, R. Li, H. Huang, S. Zhao, L. Zhang, S. Lu, C. V. Singh and X. Sun, Nano Energy , 2020, 76 , 105015. C. Wang, R. Yu, S. Hwang, J. Liang, X. Li, C. Zhao, Y. Sun, J. Wang, N. Holmes, R. Li, H. Huang, S. Zhao, L. Zhang, S. Lu, D. Su and X. Sun, Energy Storage Mater. , 2020, 30 , 98-103. C. Wang, S. Hwang, M. Jiang, J. Liang, Y. Sun, K. Adair, M. Zheng, S. Mukherjee, X. Li, R. Li, H. Huang, S. Zhao, L. Zhang, S. Lu, J. Wang, C. V. Singh, D. Su and X. Sun, Adv. Energy Mater. , 2021, 11 , 2100210. C. Wang, Y. Zhao, Q. Sun, X. Li, Y. Liu, J. Liang, X. Li, X. Lin, R. Li, K. R. Adair, L. Zhang, R. Yang, S. Lu and X. Sun, Nano Energy , 2018, 53 , 168-174. C. Wang, K. Adair and X. Sun, Acc. Mater. Res. , 2022, 3 , 21-32. C. Wang, R. Yu, H. Duan, Q. Lu, Q. Li, K. R. Adair, D. Bao, Y. Liu, R. Yang, J. Wang, S. Zhao, H. Huang and X. Sun, ACS Energy Lett. , 2022, DOI: 10.1021/acsenergylett.1c02261, 410-416. C. Wang, Q. Sun, Y. Liu, Y. Zhao, X. Li, X. Lin, M. N. Banis, M. Li, W. Li, K. R. Adair, D. Wang, J. Liang, R. Li, L. Zhang, R. Yang, S. Lu and X. Sun, Nano Energy , 2018, 48 , 35-43. C. Wang, K. R. Adair, J. Liang, X. Li, Y. Sun, X. Li, J. Wang, Q. Sun, F. Zhao, X. Lin, R. Li, H. Huang, L. Zhang, R. Yang, S. Lu and X. Sun, Adv. Funct. Mater. , 2019, 29 , 1900392.