GITT Limitations and EIS Insights into Kinetics of NMC622
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 assum...
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MDPI AG
2025-06-01
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| author | Intizar Abbas 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 Bok Hyun Ka Hoon-Hwe Cho Jongwoo Lim Namsoo Shin Miran Gaberšček Su-Mi Hur Chan-Jin Park Jaekook Kim Jong-Sook Lee |
| author_facet | Intizar Abbas 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 Bok Hyun Ka Hoon-Hwe Cho Jongwoo Lim Namsoo Shin Miran Gaberšček Su-Mi Hur Chan-Jin Park Jaekook Kim Jong-Sook Lee |
| author_sort | Intizar Abbas |
| collection | DOAJ |
| description | 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<sup>−1</sup> 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-s transients of a 10-min 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 <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi>t</mi><mo>+</mo></msub><mo>=</mo><mn>0.3</mn></mrow></semantics></math></inline-formula>, 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. |
| format | Article |
| id | doaj-art-6c673814b68e4c4893b5de5fea6f9c8a |
| institution | OA Journals |
| issn | 2313-0105 |
| language | English |
| publishDate | 2025-06-01 |
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| series | Batteries |
| spelling | doaj-art-6c673814b68e4c4893b5de5fea6f9c8a2025-08-20T02:24:39ZengMDPI AGBatteries2313-01052025-06-0111623410.3390/batteries11060234GITT Limitations and EIS Insights into Kinetics of NMC622Intizar Abbas0Huyen Tran Tran1Tran Thi Ngoc Tran2Thuy Linh Pham3Eui-Chol Shin4Chan-Woo Park5Sung-Bong Yu6Oh Jeong Lee7An-Giang Nguyen8Daeho Jeong9Bok Hyun Ka10Hoon-Hwe Cho11Jongwoo Lim12Namsoo Shin13Miran Gaberšček14Su-Mi Hur15Chan-Jin Park16Jaekook Kim17Jong-Sook Lee18School of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaBattery Diagnosis Lab, Samsung SDI, Suwon 16678, Republic of KoreaBattery Diagnosis Lab, Samsung SDI, Suwon 16678, Republic of KoreaDepartment of Materials Science and Engineering, Hanbat National University, Daejeon 34158, Republic of KoreaDepartment of Chemistry, Seoul National University, Seoul 08826, Republic of KoreaDeep Solution Inc., Seoul 06738, Republic of KoreaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaSchool of Polymer Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaSchool of Materials Science and Engineering, Chonnam National University, Gwangju 61186, Republic of KoreaConventional 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<sup>−1</sup> 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-s transients of a 10-min 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 <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi>t</mi><mo>+</mo></msub><mo>=</mo><mn>0.3</mn></mrow></semantics></math></inline-formula>, 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.https://www.mdpi.com/2313-0105/11/6/234GITTEISspherical diffusionchemical diffusivityrelaxationpulse times |
| spellingShingle | Intizar Abbas 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 Bok Hyun Ka Hoon-Hwe Cho Jongwoo Lim Namsoo Shin Miran Gaberšček Su-Mi Hur Chan-Jin Park Jaekook Kim Jong-Sook Lee GITT Limitations and EIS Insights into Kinetics of NMC622 Batteries GITT EIS spherical diffusion chemical diffusivity relaxation pulse times |
| title | GITT Limitations and EIS Insights into Kinetics of NMC622 |
| title_full | GITT Limitations and EIS Insights into Kinetics of NMC622 |
| title_fullStr | GITT Limitations and EIS Insights into Kinetics of NMC622 |
| title_full_unstemmed | GITT Limitations and EIS Insights into Kinetics of NMC622 |
| title_short | GITT Limitations and EIS Insights into Kinetics of NMC622 |
| title_sort | gitt limitations and eis insights into kinetics of nmc622 |
| topic | GITT EIS spherical diffusion chemical diffusivity relaxation pulse times |
| url | https://www.mdpi.com/2313-0105/11/6/234 |
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