Abstract
The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage technologies. Among these technologies, rechargeable aqueous zinc-ion batteries (AZIBs) have attracted considerable interest as a potential alternative to lithium-ion batteries (LIBs) due to their affordable cost, environmental compatibility and high safety standards. In this study, a high-quality electrode for AZIBs has been successfully developed using a dehydrated mixed-valence polyoxometalate-based three-dimensional (3D) inorganic framework material known as [H6Mn3VIV15VV4O46(H2O)12] (3D-MnVO). This innovative 3D-MnVO material is built from the alternate connections of {V19O46} "sphere-shaped" clusters and μ2-{Mn(H2O)4} bridges, where each {V19O46} cluster is surrounded by three pairs of vertically distributed {Mn(H2O)4} units, thus resulting in the 3D interpenetrating grid-like network from the infinite [-{V19O46}-µ2-Mn(H2O)4-{V19O46}]∞ chains in three mutually perpendicular directions. The 3D framework structure of 3D-MnVO possesses abundant oxygen vacancies, spacious and multi-level interconnected channels for ion transport, which facilitates the efficient intercalation/deintercalation of hydrated Zn2+ into the pores of the primary structure via the intercalation capacitance mechanism. As a result, the 3D-MnVO electrode exhibits excellent diffusion rates and minimal interfacial resistance. At a current density of 0.1 A·g−1, the 3D-MnVO cathode delivers a commendable discharge capacity of 170.5 mAh·g−1 with 81.6% capacity retention after 100 charge/discharge cycles. Furthermore, even at a high current density of 1.0 A·g−1, the 3D-MnVO electrode delivers a remarkable reversible capacity of 198.9 mAh·g−1. Our research results provide valuable insights into the development of advanced polyoxometalate-based 3D inorganic framework electrode materials for high-performance rechargeable AZIBs.
Graphical abstract
摘要
全球对新型能源体系的迫切需求和持续探索推动了电化学储能技术的快速发展。在这些技术中, 可充电水系锌离子电池 (AZIBs) 由于其成本低廉、环境兼容性和高安全标准等特点而引起了广泛关注, 被视为锂离子电池 (LIBs) 的潜在替代品之一。在这项研究中, 我们利用脱去结晶水的混合价多金属氧簇基三维无机框架材料[H6Mn3VIV15VV4O46(H2O)12] (3D-MnVO)作为正极材料, 开发了一种高性能水系锌离子电池电极。这种新颖的3D-MnVO材料由球形簇{V19O46}和μ2-{Mn(H2O)4}桥交替连接而成, 每个{V19O46}簇周围都有三对垂直分布的{Mn(H2O)4}单元, 从而在三个互相垂直的方向上形成了无限的{V19O46}-µ2-Mn(H2O)4-{V19O46}]∞链的三维网格结构。3D-MnVO材料的三维结构中具有丰富的氧空位、宽敞的多级互连通道, 有利于通过插层电容机制将水合锌离子高效地插入到3D-MnVO主体结构的孔隙中进行Zn2+插入/脱出反应。因此, 3D-MnVO电极具有出色的扩散速率和较小的界面电阻, 在0.1 A‧g−1的电流密度下, 3D-MnVO正极具有可观的170.5 mAh‧g−1的放电容量, 并在100次充放电循环后保持81.6%的容量保留率。此外, 即使在较高电流密度1.0 A‧g−1下, 3D-MnVO电极仍具有出色的可逆容量198.9 mAh‧g−1。我们的研究结果为开发高性能可充电水系锌电池的先进多金属氧簇基电极材料提供了宝贵的见解。
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Acknowledgements
This study was financially supported by the National Natural Science Foundation of China (Nos. 52071132, 52261135632 and U21A20284), Zhongyuan Thousand People Plan-The Zhongyuan Youth Talent Support Program (in Science and Technology), China (No. ZYQR201810139), the Natural Science Foundation of Henan, China (Nos. 232300421080 and 222300420138), the Science and Technology Project of Henan Province, China (Nos. 232102241038 and 232102241004), the Key Scientific Research Programs in Universities of Henan Province, China-Special Projects for Basic Research (No. 23ZX008), the Innovative Funds Plan of Henan University of Technology, China (No. 2020ZKCJ04), the Ph.D. Programs Foundation of Henan University of Technology, China (No. 2021BS0027), and the Doctoral Education Fund of Henan University of Engineering, China (No. DKJ2019004).
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Han, Q., Xiao, HR., Zhou, T. et al. A mixed-valence polyoxometalate-based 3D inorganic framework cathode material for high-efficiency rechargeable AZIBs. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02671-3
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DOI: https://doi.org/10.1007/s12598-024-02671-3