Enhanced dynamics of Al3+/H+ ions in aqueous aluminum ion batteries: Construction of metastable structures in vanadium pentoxide upon oxygen vacancies

IF 13.1 1区 化学 Q1 Energy Journal of Energy Chemistry Pub Date : 2024-10-22 DOI:10.1016/j.jechem.2024.09.062
Zhibao Wang, Hanqing Gu, Tianci Wu, Wenming Zhang, Zhanyu Li
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Abstract

In recent years, aqueous aluminum ion batteries have been widely studied owing to their abundant energy storage and high theoretical capacity. An in-depth study of vanadium oxide materials is necessary to address the precipitation of insoluble products covered cathode surface and the slow reaction kinetics. Therefore, a method using a simple one-step hydrothermal preparation and oxalic acid to regulate oxygen vacancies has been reported. A high starting capacity (400 mAh g−1) can be achieved by OvV2O5, and it is capable of undergoing 200 cycles at 0.4 A g−1, with a termination discharge capacity of 103 mAh g−1. Mechanism analysis demonstrated that metastable structures (AlxV2O5 and HxV2O5) were constructed through the insertion of Al3+/H+ during discharging, which existed in the lattice intercalation with V2O5. The incorporation of oxygen vacancies lowers the reaction energy barrier while improving the ion transport efficiency. In addition, the metastable structure allows the electrostatic interaction between Al3+ and the main backbone to establish protection and optimize the transport channel. In parallel, this work exploits ex-situ characterization and DFT to obtain a profound insight into the instrumental effect of oxygen vacancies in the construction of metastable structures during in-situ electrochemical activation, with a view to better understanding the mechanism of the synergistic participation of Al3+ and H+ in the reaction. This work not only reports a method for cathode materials to modulate oxygen vacancies, but also lays the foundation for a deeper understanding of the metastable structure of vanadium oxides.

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水性铝离子电池中 Al3+/H+ 离子的动力学增强:氧空位在五氧化二钒中构建可迁移结构
近年来,水性铝离子电池因其储能丰富、理论容量高而被广泛研究。要解决覆盖在阴极表面的不溶产物析出和反应动力学缓慢的问题,有必要对氧化钒材料进行深入研究。因此,一种采用简单的一步水热法制备和草酸调节氧空位的方法得到了报道。OvV2O5 可实现较高的起始容量(400 mAh g-1),并能在 0.4 A g-1 下进行 200 次循环,最终放电容量为 103 mAh g-1。机理分析表明,在放电过程中,通过插入 Al3+/H+ 构建了与 V2O5 存在晶格插层的可迁移结构(AlxV2O5 和 HxV2O5)。氧空位的加入降低了反应能垒,同时提高了离子传输效率。此外,逸散结构允许 Al3+ 与主骨架之间的静电相互作用,从而建立保护并优化传输通道。与此同时,这项工作利用原位表征和 DFT,深入了解了氧空位在原位电化学活化过程中构建陨变结构的工具效应,以期更好地理解 Al3+ 和 H+ 协同参与反应的机理。这项工作不仅报告了一种阴极材料调控氧空位的方法,而且为更深入地理解钒氧化物的陨变结构奠定了基础。
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来源期刊
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
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