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Volume 11
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Article

GITT Limitations and EIS Insights into Kinetics of NMC622

by
Intizar Abbas
1,
Huyen Tran Tran
1,
Tran Thi Ngoc Tran
1,
Thuy Linh Pham
1,
Eui-Chol Shin
1,2,
Chan-Woo Park
1,
Sung-Bong Yu
1,
Oh Jeong Lee
1,
An-Giang Nguyen
1,
Daeho Jeong
2,
Bok Hyun Ka
2,
Hoon-Hwe Cho
3,
Jongwoo Lim
4,
Namsoo Shin
5,
Miran Gaberšček
6,
Su-Mi Hur
7,
Chan-Jin Park
1,
Jaekook Kim
1 and
Jong-Sook Lee
1,*
1
School of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of Korea
2
Battery Diagnosis Lab, Samsung SDI, Suwon 16678, Republic of Korea
3
Department of Materials Science and Engineering, Hanbat National University, Daejeon 34158, Republic of Korea
4
Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea
5
Deep Solution Inc., Seoul 06738, Republic of Korea
6
Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, Slovenia
7
School of Polymer Science and Engineering, Chonnam National University, Gwangju 61186, Republic of Korea
*
Author to whom correspondence should be addressed.
Batteries 2025, 11(6), 234; https://doi.org/10.3390/batteries11060234
Submission received: 31 January 2025 / Revised: 15 May 2025 / Accepted: 16 June 2025 / Published: 19 June 2025
(This article belongs to the Section Battery Modelling, Simulation, Management and Application)
Versions Notes

Abstract

Conventional applications of the Galvanostatic Intermittent Titration Technique (GITT) and EIS for estimating chemical diffusivity in battery electrodes face issues such as insufficient relaxation time to reach equilibrium, excessively long pulse durations that violate the short-time diffusion assumption, and the assumption of sequential electrode reaction and diffusion processes. In this work, a quasi-equilibrium criterion of 0.1 mV h−1 was applied to NMC622 electrodes, yielding 8–9 h relaxations below 3.8 V, but above 3.8 V, voltage decayed linearly and indefinitely, even upon discharging titration, showing unusual nonmonotonic relaxation behavior. The initial 36-second transients of a 10-minute galvanostatic pulse and diffusion impedance in series with the electrode reaction yielded consistent diffusivity values. However, solid-state diffusion in spherical active particles within porous electrodes, where ambipolar diffusion occurs in the pore electrolyte with t+=0.3, requires a physics-based three-rail transmission line model (TLM). The corrected diffusivity may be three to four times higher. An analytic two-rail TLM approximating the three-rail numerical model was applied to temperature- and frequency-dependent EIS data. This approach mitigates parameter ambiguity and unphysical correlations in EIS. Physics-based EIS enables the identification of multistep energetics and the diagnosis of performance and degradation mechanisms.
Keywords: GITT; EIS; spherical diffusion; chemical diffusivity; relaxation; pulse times; short-time solution; three-rail transmission line model; liquid phase diffusion; transference number; temperature dependence GITT; EIS; spherical diffusion; chemical diffusivity; relaxation; pulse times; short-time solution; three-rail transmission line model; liquid phase diffusion; transference number; temperature dependence

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MDPI and ACS Style

Abbas, I.; Tran, H.T.; Tran, T.T.N.; Pham, T.L.; Shin, E.-C.; Park, C.-W.; Yu, S.-B.; Lee, O.J.; Nguyen, A.-G.; Jeong, D.; et al. GITT Limitations and EIS Insights into Kinetics of NMC622. Batteries 2025, 11, 234. https://doi.org/10.3390/batteries11060234

AMA Style

Abbas I, Tran HT, Tran TTN, Pham TL, Shin E-C, Park C-W, Yu S-B, Lee OJ, Nguyen A-G, Jeong D, et al. GITT Limitations and EIS Insights into Kinetics of NMC622. Batteries. 2025; 11(6):234. https://doi.org/10.3390/batteries11060234

Chicago/Turabian Style

Abbas, Intizar, Huyen Tran Tran, Tran Thi Ngoc Tran, Thuy Linh Pham, Eui-Chol Shin, Chan-Woo Park, Sung-Bong Yu, Oh Jeong Lee, An-Giang Nguyen, Daeho Jeong, and et al. 2025. "GITT Limitations and EIS Insights into Kinetics of NMC622" Batteries 11, no. 6: 234. https://doi.org/10.3390/batteries11060234

APA Style

Abbas, I., Tran, H. T., Tran, T. T. N., Pham, T. L., Shin, E.-C., Park, C.-W., Yu, S.-B., Lee, O. J., Nguyen, A.-G., Jeong, D., Ka, B. H., Cho, H.-H., Lim, J., Shin, N., Gaberšček, M., Hur, S.-M., Park, C.-J., Kim, J., & Lee, J.-S. (2025). GITT Limitations and EIS Insights into Kinetics of NMC622. Batteries, 11(6), 234. https://doi.org/10.3390/batteries11060234

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