Correlative Potential and Impedance Microscopy Reveals Particle-Level Degradation and Transport Heterogeneity in Solid-State Composite Cathodes
- 1National Institute of Advanced Industrial Science and Technology (AIST), 1-8-31 Midorigaoka, Ikeda, Osaka, Japan, 563-8577
Abstract
The electrochemical performance of composite cathodes in all-solid-state batteries is governed by local reaction and transport processes; however, directly linking cell-level electrochemical responses to individual activematerial particles and local microstructural features remains challenging. Here, we investigate a composite cathode in sulfide-based all-solid-state cells using correlative microscopy combining Kelvin probe force microscopy (KPFM) and scanning impedance microscopy (SIM). Following high-voltage degradation, KPFM revealed that some cathode active-material particles exhibited smaller changes in contact potential difference (CPD) between the charged and discharged states or deviations from the overall trend. Furthermore, a particle-by-particle correlation was observed between the charge–discharge CPD response and the corresponding low-frequency local AC voltage response measured by SIM. Analysis of the SIM spatial distributions using a transmission line model further provided a framework for interpreting changes in the relative contributions of electronic transport, ionic transport, and cathode active material/solid electrolyte interfacial impedance between the charged and discharged states and following high-voltage degradation. This approach provides a basis for linking particle-level reaction heterogeneity to local transport networks in composite cathodes.
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BibTeX
@misc{yamagishi2026correlative,
title = {{Correlative Potential and Impedance Microscopy Reveals Particle-Level Degradation and Transport Heterogeneity in Solid-State Composite Cathodes}},
author = {Yuji Yamagishi and Zyun Siroma and Hirotada Gamo and Yusuke Morino and Naoya Ishida and Hikaru Sano},
howpublished = {ChemRxiv},
year = {2026},
month = oct,
doi = {10.26434/chemrxiv.15009947/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009947/v1},
note = {CC BY-NC-ND},
}
RIS
TY - UNPB
TI - Correlative Potential and Impedance Microscopy Reveals Particle-Level Degradation and Transport Heterogeneity in Solid-State Composite Cathodes
AU - Yuji Yamagishi
AU - Zyun Siroma
AU - Hirotada Gamo
AU - Yusuke Morino
AU - Naoya Ishida
AU - Hikaru Sano
PY - 2026
DA - 2026/10/05
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009947/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009947/v1
AB - The electrochemical performance of composite cathodes in all-solid-state batteries is governed by local reaction and transport processes; however, directly linking cell-level electrochemical responses to individual activematerial particles and local microstructural features remains challenging. Here, we investigate a composite cathode in sulfide-based all-solid-state cells using correlative microscopy combining Kelvin probe force microscopy (KPFM) and scanning impedance microscopy (SIM). Following high-voltage degradation, KPFM revealed that some cathode active-material particles exhibited smaller changes in contact potential difference (CPD) between the charged and discharged states or deviations from the overall trend. Furthermore, a particle-by-particle correlation was observed between the charge–discharge CPD response and the corresponding low-frequency local AC voltage response measured by SIM. Analysis of the SIM spatial distributions using a transmission line model further provided a framework for interpreting changes in the relative contributions of electronic transport, ionic transport, and cathode active material/solid electrolyte interfacial impedance between the charged and discharged states and following high-voltage degradation. This approach provides a basis for linking particle-level reaction heterogeneity to local transport networks in composite cathodes.
ER -