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.
| Original language | English |
|---|---|
| Article number | 5785 |
| Journal | Nature Communications |
| Volume | 16 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2025 |
Funding
Research at Argonne National Laboratory (ANL) was supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) under the Silicon Consortium Seedling project received by Z.H.C. ANL is operated for the DOE Office of Science by UChicago Argonne, LLC, under Contract DE-AC02-06CH11357. This work at Pacific Northwest National Laboratory (PNNL) was supported by the U.S. DOE/EERE/VTO under the Advanced Battery Materials Research Program. PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. A portion of this work (Si synthesis) was performed at the Oak Ridge National Laboratory (GMV) and supported by U.S. DOE’s VTO under the Silicon Consortium Program received by G.M.V. and directed by Carine Steinway, Nicolas Eidson Thomas, Thomas Do. The authors also acknowledge the valuable discussion with team members of the Silicon Consortium Project.