DOE OSTI · 3373984
Effective Li-Ion Transport Quantification in Composite Cathodes for All-Solid-State Batteries via Multiscale Modeling and Experiments
Abstract
The tortuosity factor of composite cathodes significantly affects the rate performance of all-solid-state batteries (ASSBs) and has significant differences from systems with liquid electrolytes. Here, in this work, we report a simulation-experiment combined approach that quantifies the effective Li-ion transport in an ASSB composite cathode, which links tortuosity factor on ∼ μm scale to terminal voltage during cycling at the cell level (on ∼ cm scale). Two independent approaches of tortuosity factor quantification are considered: fitting electrochemical cycling data and verifying at different cycling rates and calculating from segmented tomography images, with the tortuosity factor quantified from both methods reaching self-consistency. The simulated terminal voltage using the quantified tortuosity factor has a small relative error of <3% compared to the experimental measurements. We find a significantly reduced value of the Bruggeman exponent of the catholyte phase (1.75), and using shape analysis, we show that rod-shaped catholyte particles play an important role in lowering the tortuosity factor.
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Yao, Archie Mingze [Univ. of Michigan, Ann Arbor, MI (United States)] (ORCID:000000016369129X), Kim, Seong-Jun [Argonne National Laboratory (ANL), Argonne, IL (United States)], Veeraraghavan, Vijay D. [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)] (ORCID:0000000173277316), Wang, Ziqi [Univ. of Michigan, Ann Arbor, MI (United States)], Gasilov, Sergey [Univ. of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.], Kastengren, Alan [Argonne National Laboratory (ANL), Argonne, IL (United States)], Chiang, Yet-Ming [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)] (ORCID:0000000208337674), Fenter, Paul [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000266729748), Viswanathan, Venkatasubramanian [Univ. of Michigan, Ann Arbor, MI (United States)] (ORCID:0000000310605495). 2025-11-13. Effective Li-Ion Transport Quantification in Composite Cathodes for All-Solid-State Batteries via Multiscale Modeling and Experiments. https://doi.org/10.1021/acs.chemmater.5c02212
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