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<p>Conventional solid electrolyte interphases (SEIs) strongly adhere to micro-silicon (µ-Si) and crack under volume changes, causing poor cycling performance. Nano-silicon improves cycling performance but remains costly with limited calendar life. Here potentiostatic ageing tests demonstrate that both calendar and cycle ageing are governed by SEI cracking and dissolution with different relative contributions. When the system is not dominated by SEI dissolution, the relative calendar life of Si anodes could correlates positively with their cycle life. LiF-rich SEI that enables long cycle life in µ-Si is therefore expected to enhance calendar life as well. Using this framework, we screened electrolytes, SEIs and electrodes and validated them with full-cell storage. LiF-rich SEI minimizes cracking and dissolution, enabling μ-Si to achieve excellent calendar life, whereas nano-silicon suffers from SEI dissolution and needs reduced electrolyte–electrode contact for better calendar life. This work clarifies calendar-ageing behaviour and accelerates electrolytes and SEI development for long-life Si anodes.</p>

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Mechanistic understanding of interphase-driven ageing in silicon anodes

  • 期刊论文

  • 发表日期：

    2026年2月3日

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  • Weiran Zhang,
  • Nan Zhang,
  • Zeyi Wang,
  • Ai-Min Li,
  • Sufu Liu,
  • Taeyong Lee,
  • Yawei Chen,
  • Yijie Liu,
  • Zheng Li,
  • Hongli Wan,
  • Sz-Chian Liou,
  • Jiancun Rao,
  • Joseph Roschella,
  • Lei Zheng,
  • Zhiyuan Zhang,
  • Huixin He,
  • Brett L. Lucht,
  • Christopher S. Johnson,
  • Chunsheng Wang

摘要

Conventional solid electrolyte interphases (SEIs) strongly adhere to micro-silicon (µ-Si) and crack under volume changes, causing poor cycling performance. Nano-silicon improves cycling performance but remains costly with limited calendar life. Here potentiostatic ageing tests demonstrate that both calendar and cycle ageing are governed by SEI cracking and dissolution with different relative contributions. When the system is not dominated by SEI dissolution, the relative calendar life of Si anodes could correlates positively with their cycle life. LiF-rich SEI that enables long cycle life in µ-Si is therefore expected to enhance calendar life as well. Using this framework, we screened electrolytes, SEIs and electrodes and validated them with full-cell storage. LiF-rich SEI minimizes cracking and dissolution, enabling μ-Si to achieve excellent calendar life, whereas nano-silicon suffers from SEI dissolution and needs reduced electrolyte–electrode contact for better calendar life. This work clarifies calendar-ageing behaviour and accelerates electrolytes and SEI development for long-life Si anodes.