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<p>All-solid-state lithium metal batteries promise high levels of safety and energy density, but their practical realization is limited by low Li reversibility, limited cell loading and demand for high-temperature and high-pressure operation, stemming from solid-state electrolyte (SSE) low-voltage reduction and high-voltage decomposition, and from lithium dendrite growth. Here we concurrently address these challenges by reporting that a family of reductive electrophiles gain electrons and cations from metal–nucleophile materials (here a Li sulfide SSE) upon contact to undergo electrochemical reduction and form interphase layers (named solid reductive-electrophile interphase) on material surfaces. The solid reductive-electrophile interphase is electron blocking and lithiophobic, prevents SSE reduction, suppresses Li dendrites and supports high-voltage cathodes. Consequently, a reductive-electrophile-treated SSE exhibits high critical capacity and Li reversibility at the anode, and enables Li(1% Mg)/SSE/LiNi<sub>0.8</sub>Co<sub>0.15</sub>Al<sub>0.05</sub>O<sub>2</sub> all-solid-state lithium metal batteries to achieve a high coulombic efficiency (&gt;99.9%), long cycle life (~10,000 h) and high loading (&gt;7 mAh cm<sup>−2</sup>) at 30 °C and 2.5 MPa. This concept also extends to cathodes of other materials (for example, metal oxides), boosting the high-nickel cathode’s cycle life and expanding the operational voltage up to 4.5 V. Such solid reductive-electrophile interphase tailoring of material surfaces holds promise to accelerate all-solid-state lithium metal battery commercialization and offer solutions for a wide range of materials.</p>

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Revitalizing interphase in all-solid-state Li metal batteries by electrophile reduction

  • 期刊论文

  • 发表日期：

    2025年1月20日

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  • Weiran Zhang,
  • Zeyi Wang,
  • Hongli Wan,
  • Ai-Min Li,
  • Yijie Liu,
  • Sz-Chian Liou,
  • Kai Zhang,
  • Yuxun Ren,
  • Chamithri Jayawardana,
  • Brett L. Lucht,
  • Chunsheng Wang

摘要

All-solid-state lithium metal batteries promise high levels of safety and energy density, but their practical realization is limited by low Li reversibility, limited cell loading and demand for high-temperature and high-pressure operation, stemming from solid-state electrolyte (SSE) low-voltage reduction and high-voltage decomposition, and from lithium dendrite growth. Here we concurrently address these challenges by reporting that a family of reductive electrophiles gain electrons and cations from metal–nucleophile materials (here a Li sulfide SSE) upon contact to undergo electrochemical reduction and form interphase layers (named solid reductive-electrophile interphase) on material surfaces. The solid reductive-electrophile interphase is electron blocking and lithiophobic, prevents SSE reduction, suppresses Li dendrites and supports high-voltage cathodes. Consequently, a reductive-electrophile-treated SSE exhibits high critical capacity and Li reversibility at the anode, and enables Li(1% Mg)/SSE/LiNi0.8Co0.15Al0.05O2 all-solid-state lithium metal batteries to achieve a high coulombic efficiency (>99.9%), long cycle life (~10,000 h) and high loading (>7 mAh cm−2) at 30 °C and 2.5 MPa. This concept also extends to cathodes of other materials (for example, metal oxides), boosting the high-nickel cathode’s cycle life and expanding the operational voltage up to 4.5 V. Such solid reductive-electrophile interphase tailoring of material surfaces holds promise to accelerate all-solid-state lithium metal battery commercialization and offer solutions for a wide range of materials.