(Invited) Developing High-Energy All-Solid-State Batteries with Long Cycle Life

Abstract

While conventional lithium-ion batteries (LIBs) continue to gain progress through incremental improvements, the presence of organic liquid electrolytes brings about fundamental safety issues as their reactivity and flammability subject LIBs to thermal runaway. [1-4] With higher energy densities and better safety performances, all-solid-state batteries (ASSBs) consisting of a 4 V-class cathode active material (CAM), an inorganic solid-state electrolyte (SE) and a lithium-metal anode are considered the future of energy storage technologies. [5-6] The development of practical ASSBs, however, has met a number of challenges. SEs simultaneously meeting the criteria in conductivity, stability and mechanical properties are yet to be discovered. At the anode, reductive degradation of SE, high interfacial impedance and dendrite formation are the most pressing issues. At the cathode, instabilities due to oxidative degradation of SE, reactivities between SE and CAM as well as the loss of mechanical integrity significantly limit ASSB performance.In this presentation, we discuss our recent effort in addressing these challenges, including the development of novel halide SEs, design of composite cathode structure that enables direct use of uncoated-LiNi0.8Co0.1Mn0.1O2 CAM, and implement of Li-metal based anodes that enable better interface with the SE. We demonstrate the excellent long-term cycling performance achieved on such cells and illustrate the underlying working mechanism. [7] The importance in proper matching of cathode, SE and anode properties as well as our views on future development of better-performing ASSB cells will be presented. References Arbizzani, G. Gabrielli and M. Mastragostino, Journal of Power Sources, 2011, 196, 4801-4805.Murmann, R. Schmitz, S. Nowak, N. Ignatiev, P. Sartori, I. Cekic-Laskovic and M. Winter, Journal of The Electrochemical Society, 2015, 162, A1738.Cao, X. Ren, L. Zou, M. H. Engelhard, W. Huang, H. Wang, B. E. Matthews, H. Lee, C. Niu and B. W. Arey, Nature Energy, 2019, 4, 796-805.Fan, L. Chen, O. Borodin, X. Ji, J. Chen, S. Hou, T. Deng, J. Zheng, C. Yang, S.-C. Liou, K. Amine, K. Xu and C. Wang, Nature Nanotechnology, 2018, 13, 715-722.Janek and W. G. J. N. E. Zeier, Nature Energy, 2016, 1, 1-4.Famprikis, P. Canepa, J. A. Dawson, M. S. Islam and C. Masquelier, Nature Materials, 2019, 18, 1278-1291.Y. Kim, H. Cha, R. Kostecki and G. Chen, ACS Energy Letters 2023, 8, 521.