Deciphering coulombic loss in lithium-ion batteries and beyond

Jiyu Cai, Steve E. Trask, Zhenzhen Yang, Yingying Xie, Wenquan Lu, Hoai Nguyen, Yuzi Liu, Xiangbo Meng, Gabriel M. Veith, Hao Jia, Wu Xu and Zonghai Chen ()
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Jiyu Cai: Argonne National Laboratory
Steve E. Trask: Argonne National Laboratory
Zhenzhen Yang: Argonne National Laboratory
Yingying Xie: Argonne National Laboratory
Wenquan Lu: Argonne National Laboratory
Hoai Nguyen: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
Xiangbo Meng: University of Arkansas
Gabriel M. Veith: Oak Ridge National Laboratory
Hao Jia: Pacific Northwest National Laboratory
Wu Xu: Pacific Northwest National Laboratory
Zonghai Chen: Argonne National Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Lithium-ion batteries are pivotal for modern energy storage, yet accurately predicting their lifespan remains a critical challenge. While descriptors like coulombic efficiency are widely used to assess battery longevity, the unclear physical origins of coulombic losses cause semi-quantitative correlation with capacity, complicating battery development. Here, we combine high-precision leakage current and open-circuit-voltage measurements with charge conservation principles to explore microscopic charge consumptions at electrode-electrolyte interfaces across diverse chemistries. We demonstrate that coulombic loss arises from a synergy between local charge neutrality and global charge compensation, reconciling its quantitative correlation to capacity. Contrary to conventional assumptions equating coulombic loss with irreversible capacity loss, this framework resolves systematic overestimations and paradoxical phenomena in existing chemistries. Our findings establish physics-informed criteria for accelerated lifespan evaluation and guide rational design of long-life lithium-ion batteries and beyond.

Date: 2025
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DOI: 10.1038/s41467-025-60833-y

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