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

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., Li4Ti5O12, TiNb2O7) operate at high potentials (>1.5 V vs. Li+/Li) to circumven...

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Main Authors: 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
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61461-2
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Summary: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., 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.
ISSN:2041-1723