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<p>Developing lithium-ion batteries with high specific energy and fast-charging capability requires overcoming the potential-capacity trade-off in negative electrodes. Conventional fast-charging materials (e.g., Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub>, TiNb<sub>2</sub>O<sub>7</sub>) operate at high potentials (&gt;1.5 V vs. Li<sup>+</sup>/Li) to circumvent lithium plating, yet this compromises specific energy. A viable strategy for enhancing the specific energy is to reduce the potential while avoiding the lithium plating risk; however, the underlying mechanisms remain unclear. Here we demonstrate that enhancing Titanium-Oxygen covalency through pseudo-Jahn-Teller Effect distortion in Ruddlesden-Popper perovskites enables low-potential operation. The Li<sub>2</sub>La<sub>2</sub>Ti<sub>3</sub>O<sub>10</sub> negative electrode exhibits a working potential of 0.5 V vs. Li<sup>+</sup>/Li with initial 139.3 mAh g<sup>−1</sup> at 5 A g<sup>−1</sup> and 72.9% capacity retention after 5000 cycles. Full cells with LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> positive electrodes deliver 3.45 V average discharge voltage-50% higher than conventional Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> | |LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> systems-achieving 100 mAh g<sup>−1</sup> at 4 A g<sup>−1</sup>. Mechanistic analysis reveals low Li⁺ migration barriers and stable Ruddlesden-Popper perovskite frameworks enable rapid ion transport.</p>

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Enhanced specific energy in fast-charging lithium-ion batteries negative electrodes via Ti-O covalency-mediated low potential

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月7日

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  • Jun Huang,
  • Qirui Yang,
  • Anyi Hu,
  • Zhu Liao,
  • Zhengxi Zhang,
  • Qinfeng Zheng,
  • Zhouhong Ren,
  • Shun Zheng,
  • Yixiao Zhang,
  • Xiaolong Yang,
  • Zhenming Xu,
  • Le Zhang,
  • Daming Zhu,
  • Wen Wen,
  • Xi Liu,
  • Akihiro Orita,
  • Nagahiro Saito,
  • Liguang Wang,
  • Yongyao Xia,
  • Liwei Chen,
  • Jun Lu,
  • Li Yang

摘要

Developing lithium-ion batteries with high specific energy and fast-charging capability requires overcoming the potential-capacity trade-off in negative electrodes. Conventional fast-charging materials (e.g., Li4Ti5O12, TiNb2O7) operate at high potentials (>1.5 V vs. Li+/Li) to circumvent lithium plating, yet this compromises specific energy. A viable strategy for enhancing the specific energy is to reduce the potential while avoiding the lithium plating risk; however, the underlying mechanisms remain unclear. Here we demonstrate that enhancing Titanium-Oxygen covalency through pseudo-Jahn-Teller Effect distortion in Ruddlesden-Popper perovskites enables low-potential operation. The Li2La2Ti3O10 negative electrode exhibits a working potential of 0.5 V vs. Li+/Li with initial 139.3 mAh g−1 at 5 A g−1 and 72.9% capacity retention after 5000 cycles. Full cells with LiNi0.8Co0.1Mn0.1O2 positive electrodes deliver 3.45 V average discharge voltage-50% higher than conventional Li4Ti5O12 | |LiNi0.8Co0.1Mn0.1O2 systems-achieving 100 mAh g−1 at 4 A g−1. Mechanistic analysis reveals low Li⁺ migration barriers and stable Ruddlesden-Popper perovskite frameworks enable rapid ion transport.