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<p>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.</p>

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Deciphering coulombic loss in lithium-ion batteries and beyond

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年7月1日

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  • Jiyu Cai,
  • Steve E. Trask,
  • Zhenzhen Yang,
  • Yingying Xie,
  • Wenquan Lu,
  • Hoai Nguyen,
  • Yuzi Liu,
  • Xiangbo Meng,
  • Gabriel M. Veith,
  • Hao Jia,
  • Wu Xu,
  • Zonghai Chen

摘要

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.