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

Huang, Jun; Yang, Qirui; Hu, Anyi; Liao, Zhu; Zhang, Zhengxi; Zheng, Qinfeng; Ren, Zhouhong; Zheng, Shun et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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 (>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.