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Oxygen-deficient ammonium vanadate/GO composites with suppressed vanadium dissolution for ultra-stable high-rate aqueous zinc-ion batteries

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Abstract

The structural engineering of hydrated ammonium vanadate as a cathode for aqueous Zn-ion batteries has attracted significant research interest because of its ability to suppress vanadium dissolution and accelerate the electrochemical dynamics. Herein, a feasible fabrication strategy for oxygen-deficient (NH4)2V10O25·xH2O/GO (NVOH@GO) composites was proposed, and the charge storage mechanism was discussed. The results of characterization analysis showed that the introduction of graphene oxide (GO) not only enlarged the layer spacing and improved electrical conductivity, providing spacious channels for Zn2+ (de)intercalation and accelerating the ion diffusion dynamics, but also induced more oxygen vacancies, inhibited the dissolution of vanadium, and reduced self-discharging, offering additional and stable active sites for ion storage. The optimized NVOH@GO electrode delivered extraordinarily stable capacities of 334 mAh·g−1 after 2000 cycles at 5 A·g−1 and 238 mAh·g−1 after 10,000 cycles at 20 A·g−1. Furthermore, ex-situ X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman results systematically revealed the electrochemical mechanism, including a phase transition reaction and subsequent Zn2+/H2O co-(de)intercalation process. This study provides an effective strategy for expanding the interlayer spacing, inducing defect engineering, and enhancing the structural stability of vanadium-based cathodes for Zn-ion batteries and other multivalent aqueous ion batteries.

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摘要

作为水系锌离子电池的正极材料, 水合钒酸铵能够抑制钒溶解、加速电化学动力学, 因此, 其结构工程研究引起了广泛的研究兴趣。本文, 我们提出了一种缺氧(NH4)2V10O25∙xH2O/GO (NVOH@GO)复合材料的制备策略, 并探讨了其电荷存储机制。表征结果表明, 氧化石墨烯(GO)的引入, 不仅扩大了层间距、提高了导电性, 为Zn2+(脱)插层提供了更宽敞的通道、加快了离子扩散动力学; 而且诱导产生了更多氧空位、抑制了钒的溶解、降低了自放电, 为离子存储提供了稳定的活性位点。优化的NVOH@GO电极在5 A·g−1循环2000次、20 A·g−1循环10,000次后, 分别具有334和238 mAh·g−1的稳定容量。此外, 非原位X射线衍射、X射线光电子能谱和拉曼结果, 系统地揭示了其电化学机制, 包括相变反应和Zn2+/H2O共(脱)插层过程。本文提供了一种具有较大层间距、丰富缺陷和较强结构稳定性的锌离子电池和其他多价水离子电池用钒基正极的制备策略。

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Acknowledgements

This study was financially supported by the Natural Science Foundations of China (Nos. 51904152 and 42002040), Natural Science Foundations of Henan Province (No. 222300420502), Key Science and Technology Program of Henan Province (No. 222102240044), and Key Scientific Research Projects in Colleges and Universities of Henan Province (No. 21B610010).

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  1. Gui-Long Liu and Ting Zhang have contributed equally to this work.

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  1. Key Laboratory of Function-Oriented Porous Materials of Henan Province, College of Chemistry and Chemical Engineering, Luoyang Normal University, Luoyang, 471934, China

    Gui-Long Liu, Ting Zhang, Xiao-Jie Li, Ru-Ping Cao, Jin-Ke Shen, Dong-Lei Guo, Nai-Teng Wu, Wei-Wei Yuan & Xian-Ming Liu

  2. Department of Physics, Technical University of Denmark, Kongens Lyngby, 2800, Denmark

    Ang Cao

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Liu, GL., Zhang, T., Li, XJ. et al. Oxygen-deficient ammonium vanadate/GO composites with suppressed vanadium dissolution for ultra-stable high-rate aqueous zinc-ion batteries. Rare Met. 42, 3729–3740 (2023). https://doi.org/10.1007/s12598-023-02364-3

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