Utilization Ratio of Active Materials in All-Solid-State Batteries Examined Using Electrochemical Impedance Analysis with the Transmission Line Model

Abstract

In all-solid-state batteries (ASSB), increasing the thickness of electrodes is essential for increasing the energy density. However, this limits the C-rate performance, particularly for electrodes with a large volume fraction of active materials (AMs), transport of ions in the electrode is hindered, leading to poor utilization of AMs in ASSBs. To accelerate the development of ASSBs, it is highly desirable to develop analytical methods for understanding the utilization of AMs in thick electrodes. In this paper, we propose a novel impedance analysis method using the transmission line model (TLM) for estimating the utilization of AMs in an electrode in terms of effective electrode thickness. In the TLM model, electrode thickness is treated as a variable instead of a fixed parameter in the conventional sequence. Hence, the modified C-rate performance considering the TLM-calculated thickness exhibits an identical trend regardless of the actual electrode thickness, suggesting the calculated electrode thickness reflects the effective electrode thickness. This indicates effective utilization of AMs for electrochemical reactions. We also demonstrate the versatility of this method by using different electrode specifications.