Probing Formation, Degradation, and Entropic Changes in Lithium-Ion Batteries Via a Versatile Reference Electrode
Abstract
In 2013, Wenquan Lu and colleagues at Argonne National Lab proposed entropy coefficient as a parameter that could characterize the structural changes in lithium and manganese rich (LMR) layered transition metal oxide cathode active materials as voltage fade progresses over life. Subsequently, in 2021, Friedrich and Gasteiger demonstrated entropic changes between the first activation cycle of LRM-NCM and subsequent stabilization cycle. The work seen here demonstrates entropy coefficient as a parameter that tracks structural changes in LMR active materials as voltage fade progresses over life through the use of a versatile reference electrode placed between a graphite anode and LMR cathode. The entropy coefficient of the LMR and graphite are measured explicitly using the versatile reference electrode at three different points during an accelerated degradation study, illustrating the change in the entropy coefficient and associated equilibrium potential shift in the materials due to structural changes. Additionally, by activating the reference electrode (partially delithiating it to the plateau potential) prior to cell formation, the performance of each electrode during the formation process can be studied, offering a picture into first cycle efficiency in-situ.
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BibTeX
@misc{koch2026probing,
title = {{Probing Formation, Degradation, and Entropic Changes in Lithium-Ion Batteries Via a Versatile Reference Electrode}},
author = {Brian Koch and Jing Gao and Taylor R. Garrick},
howpublished = {ECSarXiv},
year = {2026},
month = sep,
doi = {10.1149/osf.io/9z7kj_v1},
url = {https://osf.io/preprints/ecsarxiv/9z7kj_v1/},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Probing Formation, Degradation, and Entropic Changes in Lithium-Ion Batteries Via a Versatile Reference Electrode
AU - Brian Koch
AU - Jing Gao
AU - Taylor R. Garrick
PY - 2026
DA - 2026/09/13
PB - ECSarXiv
DO - 10.1149/osf.io/9z7kj_v1
UR - https://osf.io/preprints/ecsarxiv/9z7kj_v1/
AB - In 2013, Wenquan Lu and colleagues at Argonne National Lab proposed entropy coefficient as a parameter that could characterize the structural changes in lithium and manganese rich (LMR) layered transition metal oxide cathode active materials as voltage fade progresses over life. Subsequently, in 2021, Friedrich and Gasteiger demonstrated entropic changes between the first activation cycle of LRM-NCM and subsequent stabilization cycle. The work seen here demonstrates entropy coefficient as a parameter that tracks structural changes in LMR active materials as voltage fade progresses over life through the use of a versatile reference electrode placed between a graphite anode and LMR cathode. The entropy coefficient of the LMR and graphite are measured explicitly using the versatile reference electrode at three different points during an accelerated degradation study, illustrating the change in the entropy coefficient and associated equilibrium potential shift in the materials due to structural changes. Additionally, by activating the reference electrode (partially delithiating it to the plateau potential) prior to cell formation, the performance of each electrode during the formation process can be studied, offering a picture into first cycle efficiency in-situ.
ER -