EXTENDED ABSTRACT: The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy. In this context, solid-state lithium batteries emerge as promising candidates to fulffll the requirements by substituting liquid electrolytes with solid-state electrolytes (SSEs). However, conventional inorganic solid electrolytes and polymer solid electrolytes have encountered limitations stemming from poor interfacial compatibility and low ionic conductivity, respectively. To circumvent the challenge, novel electrolyte systems have been explored, including composite solid electrolytes formed by combining inorganic ffllers with polymer, and quasi-solid state electrolytes achieved formed by integrating organic solvents into solid electrolyte matrices. To propel the evolution of solid electrolyte design, a more comprehensive understanding of ion transport behavior and the formulation of innovative design strategies are imperative. By employing a hybrid theoretical and experimental approach, we have identiffed solvent-assisted hopping as the predominant pathway for Li+ conduction within intrinsically anionic metal–organic framework (MOF)-based quasi-solid-state electrolytes. Furthermore, we have developed design strategies aimed at regulating the local environment at the interface between inorganic ffllers and the polymer phase within composite electrolytes, thereby achieving enhanced ionic conductivity and prolonged battery cycling. Keywords：Solid-state electrolyte; multi-scale modeling REFERENCES: [1] Guo, S.‡; Tan, S.‡; Ma, J.; Chen, L.; Yang, K.; Zhu, Q.; Ma, Y.; Shi, P.; Wei, Y.; An, X.; Ren, Q.; Huang, Y.; Zhu, Y.; Cheng, Y.; Lv, W.; Hou, T.*; Liu, M.*; He, Y.*; Yang, Q.; Kang, F.* Dissociation mechanism of lithium salt by BaTiO3 with spontaneous polarization. Energy Environ. Sci. 2024, 17, 3797–3806. [2] Zhu, Y.‡; Lao, Z.‡; Zhang, M.‡; Hou, T.*; Xiao, X.; Piao, Z.; Lu, G.; Han, Z.; Gao, R.; Nie, L.; Wu, X.; Song, Y.; Ji, C.; Wang, J.; Zhou, G.* A locally solvent-tethered polymer electrolyte for ultra-long-life lithium metal batteries. Nat. Commun. 2024, 15, 3914. [3] Hou, T.‡; Xu, W.‡; Pei, X.; Jiang, L.; Yaghi, O. M.*; Persson, K. A.* Ionic Conduction Mechanism and Design of Metal– Organic Frameworks Based Quasi-Solid-State Electrolytes. J. Am. Chem. Soc. 2022, 144, 13446-13450.
Dr. Tingzheng Hou is an Assistant Professor at the Institute of Materials Research at Tsinghua Shenzhen International Graduate School. He received his Ph.D. in Materials Science and Engineering from the University of California, Berkeley in 2021. Following his doctoral study, he worked as a postdoctoral scholar at UC Berkeley until 2022. He obtained his M.S. in Chemical Engineering in 2016 and his B.S. in Materials Science and Engineering in 2014 from Tsinghua University. His research focuses on the computational modeling and rational design of novel energy storage materials, the development of high throughput computational infrastructures, and the application of artiffcial intelligence in materials research. He has authored or co-authored 29 refereed research papers with a total citation of over 7,000. He has been awarded the First-class Natural Science Award by China Ministry of Education (2019) and the China Top Cited Author Award from IOP Publishing (2018). He actively contributes to the Materials Project as a core developer. He serves an Early-Career Editorial Board member of Energy Mater. Devices, and an invited peer reviewer for Nat. Catal., Nat. Commun., J. Am. Chem. Soc., Adv. Funct. Mater., etc.