Cross-Dataset Assessment of Cathode Thermal Descriptors for Whole-Cell Self-Heating Kinetics in Lithium-Ion Batteries: Onset, Reaction Magnitude, and Limits of Transferability
- 1School of Energy and Mechanical Engineering, Dezhou University, Dezhou 253023, China
- 2School of Mechanical Engineering, Dalian Jiaotong University, Dalian 116028, China
- 3School of Materials Science and Engineering, Dalian University of Technology, Dalian 116024, China
Abstract
Component calorimetry is widely used to assess the thermal stability of lithium-ion battery cathode materials, yet it remains unclear which material-scale descriptors retain consistent relationships with whole-cell self-heating kinetics across independent datasets and test protocols. Here, raw accelerating rate calorimetry (ARC) and thermogravimetric/differential scanning calorimetry (TGA/DSC) data for lithium cobalt oxide (LCO), lithium iron phosphate (LFP), and nickel–cobalt–aluminum oxide (NCA) cells were reanalyzed using a physics-guided event framework. Cathode decomposition onset, event-specific apparent exothermic energy, and associated mass loss were compared with the maximum whole-cell self-heating rate. In the Sandia dataset, cathode onset and event-specific exothermic energy showed large matched-state-of-charge correlations with whole-cell self-heating kinetics (r = −0.983 and 0.980, respectively). In an independently generated dataset, the cathode–electrolyte onset relationship was substantially weaker (r = −0.376), whereas cathode–electrolyte reaction enthalpy retained a large association (r = 0.886). Rank-based sensitivity analysis preserved this contrast, whereas leave-one-chemistry-out stress tests were unstable for all three Sandia linear models, indicating that the strong within-dataset associations did not extrapolate reliably to an unseen chemistry. Because the two heat-release metrics were obtained under different sample configurations and calorimetric protocols, the cross-study comparison is interpreted at the descriptor-class level rather than as direct metric equivalence. Across the two conventional lithium-ion datasets examined, cathode-associated exothermic magnitude showed greater cross-dataset consistency than onset temperature alone. However, neither descriptor supported a universal chemistry-independent scaling law, indicating that component-to-cell relationships remain dependent on experimental protocol, electrode interactions, cell architecture, and battery platform.
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BibTeX
@article{li2026crossdataset,
title = {{Cross-Dataset Assessment of Cathode Thermal Descriptors for Whole-Cell Self-Heating Kinetics in Lithium-Ion Batteries: Onset, Reaction Magnitude, and Limits of Transferability}},
author = {Yuanzhe Li and Ningning Wei and Minghai Li and Lei Huo},
journal = {Batteries},
year = {2026},
month = oct,
doi = {10.3390/batteries12100421},
url = {https://www.mdpi.com/2313-0105/12/10/421},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Cross-Dataset Assessment of Cathode Thermal Descriptors for Whole-Cell Self-Heating Kinetics in Lithium-Ion Batteries: Onset, Reaction Magnitude, and Limits of Transferability
AU - Yuanzhe Li
AU - Ningning Wei
AU - Minghai Li
AU - Lei Huo
PY - 2026
DA - 2026/10/12
JO - Batteries
DO - 10.3390/batteries12100421
UR - https://www.mdpi.com/2313-0105/12/10/421
AB - Component calorimetry is widely used to assess the thermal stability of lithium-ion battery cathode materials, yet it remains unclear which material-scale descriptors retain consistent relationships with whole-cell self-heating kinetics across independent datasets and test protocols. Here, raw accelerating rate calorimetry (ARC) and thermogravimetric/differential scanning calorimetry (TGA/DSC) data for lithium cobalt oxide (LCO), lithium iron phosphate (LFP), and nickel–cobalt–aluminum oxide (NCA) cells were reanalyzed using a physics-guided event framework. Cathode decomposition onset, event-specific apparent exothermic energy, and associated mass loss were compared with the maximum whole-cell self-heating rate. In the Sandia dataset, cathode onset and event-specific exothermic energy showed large matched-state-of-charge correlations with whole-cell self-heating kinetics (r = −0.983 and 0.980, respectively). In an independently generated dataset, the cathode–electrolyte onset relationship was substantially weaker (r = −0.376), whereas cathode–electrolyte reaction enthalpy retained a large association (r = 0.886). Rank-based sensitivity analysis preserved this contrast, whereas leave-one-chemistry-out stress tests were unstable for all three Sandia linear models, indicating that the strong within-dataset associations did not extrapolate reliably to an unseen chemistry. Because the two heat-release metrics were obtained under different sample configurations and calorimetric protocols, the cross-study comparison is interpreted at the descriptor-class level rather than as direct metric equivalence. Across the two conventional lithium-ion datasets examined, cathode-associated exothermic magnitude showed greater cross-dataset consistency than onset temperature alone. However, neither descriptor supported a universal chemistry-independent scaling law, indicating that component-to-cell relationships remain dependent on experimental protocol, electrode interactions, cell architecture, and battery platform.
SN - 2313-0105
ER -