Solid-state batteries provide a promising alternative to Li-ion batteries with improved energy density, safety, and manufacturability. However, anode-free cell configurations still suffer from multiple shortcomings, including 1) nonuniform Li deposition and dissolution, 2) continual formation of a solid-electrolyte interphase (SEI), and 3) limited rate capability. Recent efforts have investigated the integration of a carbon/silver composite interlayer to address the aforementioned challenges [1]; however, complete understanding of the mechanisms of this improved performance is not fully understood. The type of carbon, metal alloy, and lithiation effects of these components have been investigated [2,3], particularly, the electrochemical characteristics, but the mechanical properties of these interlayers have not been thoroughly investigated. Therefore, in this study we explore the interfacial mechanics at an amorphous carbon interlayer and argyrodite solid electrolyte interface on in situ Li metal formation.The carbon interlayer and solid electrolyte interfacial adhesion were modified to investigate the corresponding influence on Li metal deposition. Peel tests are performed to quantify the interlayer adhesion under various processing conditions. Li metal was observed to preferentially deposit at regions with the lowest energy penalty for nucleation and growth. By intentionally tuning the carbon/solid electrolyte interface, the growth of Li metal can be promoted at different interfaces. Operando video microscopy and post-mortem focused ion-beam/scanning electron microscopy were utilized to confirm the Li deposition behavior. This work demonstrates that Li deposition in the presence of a carbon interlayer can be systematically modified by tuning the interfacial mechanics. The outcomes of this study will further our understanding of the processing conditions and underlying mechanics during in situ Li metal formation to enable high efficacy interlayers in solid-state batteries.[1] Y.G. Lee, S. Fujiki, C. Jung, N. Suzuki, N. Yashiro, R. Omoda, D. S. Ko, T. Shiratsuchi, T. Sugimoto, S. Ryu, J. H. Ku, T. Watanabe, Y. Park, Y. Aihara, D. Im, I. T. Han, Nature Energy. 5, 299-308 (2020)[2] D.W. Liao, T.H. Cho, S. Sarna, M.K. Jangid, H. Kawakami, T. Kotaka, K. Aotani, N.P. Dasupta, Journal of Materials Chemistry A, 12, 5990-6003 (2024)[3] N. Suzuki, N. Yashiro, S. Fujiki, R. Omoda, T. Shiratsuchi, T. Watanabe, Y. Aihara, Advanced Energy and Sustainability Research, 2, 2100066 (2021)
Read full abstract