Delocalized electronic engineering of TiNb<sub>2</sub>O<sub>7</sub> enables low temperature capability for high-areal-capacity lithium-ion batteries.

Zhang, Yan; Wang, Yingjie; Zhao, Wei; Zuo, Pengjian; Tong, Yujin; Yin, Geping; Zhu, Tong; Lou, Shuaifeng · Nat Commun · 2024

basic_science · Level V

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Abstract

High areal capacity and low-temperature ability are critical for lithium-ion batteries (LIBs). However, the practical operation is seriously impeded by the sluggish rates of mass and charge transfer. Herein, the active electronic states of TiNb<sub>2</sub>O<sub>7</sub> material is modulated by dopant and O-vacancies for enhanced low-temperature dynamics. Femtosecond laser-based transient absorption spectroscopy is employed to depict carrier dynamics of TiNb<sub>2</sub>O<sub>7</sub>, which verifies the localized structure polarization accounting for reduced transport overpotential, facilitated electron/ion transport, and improved Li<sup>+</sup> adsorption. At high-mass loading of 10 mg cm<sup>-2</sup> and -30 °C, TNO<sub>-x</sub>@N microflowers exhibit stable cycling performance with 92.9% capacity retention over 250 cycles at 1 C (1.0-3.0 V, 1 C = 250 mA g<sup>-1</sup>). Even at -40 °C, a competitive areal capacity of 1.32 mAh cm<sup>-2</sup> can be achieved. Such a fundamental understanding of the intrinsic structure-function put forward a rational viewpoint for designing high-areal-capacity batteries in cold regions.