Abstract

All-solid-state lithium batteries (ASSLBs) have gained intensive attention because of their intrinsic safety and high energy density.1 However, significant interfacial challenges such as detrimental interfacial reactions, poor solid-solid ionic contact, and lithium dendrite growth have stymied the development of ASSLBs. Besides that, the large gap between fundamental research and practical engineering design has slowed down ASSLBs commercialization. Over the past five years, our group has been dedicated to the research and development of ASSLBs, with the aims of overcoming the interfacial challenges and pushing ASSLBs closer to commercialization. First, we have regulated the interfacial ion and electron transport via increasing the ionic conductivity of interfacial buffer layers,2 manipulating interfacial nanostructures,3, 4 using single-crystal cathodes,5 deciphering interfacial reaction mechanisms,6 and constructing artificial solid electrolyte interphases (SEI).7 Based on these advanced and innovative strategies, the large interfacial resistance was successfully eliminated. As a result, ASSLBs with sulfide electrolytes demonstrated both ultra-long cycling stability and high-rate performance. To transfer these viable technologies into practical application and bridging the large gap between laboratory research and practical full cells, we are committed to engineering solid-state pouch cells with competitive energy density and low cost. Recently, a solvent-free and cost-effective process was developed for fabricating ultra-thin inorganic solid electrolyte membranes as well as solid-state thick electrodes. Furthermore, a solid-liquid interface and a plastic crystal electrolyte were engineered to enable practical solid-state pouch cells with high energy density and excellent safety.8, 9 These works not only provide an in-depth understanding of interfacial mass and charge transport but also offer feasible strategies to commercialize practical solid-state pouch cells. References C. Wang, J. Liang, Y. Zhao, M. Zheng, X. Li, X. Sun*, Energy Environ. Sci. , 2021, doi:10.1039/d1ee00551k.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, X. Sun*. Adv. Energy Mater., 2021, 2100210. doi:10.1002/aenm.202100210.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, 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.

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