Abstract
Metal chalcogenide compounds can be used as high-performance cathodes for aqueous Zn batteries. However, the low accessible surfaces and violent volumetric expansion limit their properties and applications. To address these, phase-engineering strategies coupled with a hollow structure were applied to regulate the adsorption/desorption of OH− on the electrode surface and enhance the electrochemical performance. In this study, using a Se@C nanorod template, a series of carbon nanotube (CNT)-supported nickel selenides, including cubic NiSe2, NiSe2/Ni0.85Se composites, and hexagonal Ni0.85Se, were synthesized through an in situ selenylation process for the first time. Due to the large specific surface, high porosity, and hollow carbon skeleton, the optimized NiSe2/Ni0.85Se/CNT has a high specific capacity of 616 Cg−1, excellent rate capability, and stable cycling performance. In addition, its inside Faradic mechanism was investigated using a series of ex situ characterizations and density functional theory calculations. Thus, the fabricated Ni//Zn battery presents a high energy density of 311.4 W h kg−1 at 3485 W kg−1 and long cycling life. This study offers an ingenious strategy for designing nickel selenide electrodes and deeper perception for its Faradic mechanism in alkaline Zn battery.
摘要
金属硫系化合物作为水相锌电池的高性能阴极具有很大的潜力.然而, 低可达表面和剧烈的体积膨胀限制了其整体性能和实际应用. 为此, 采用相工程策略结合空心结构设计, 调控OH−在电极表面的吸附/脱附, 能显著提高电极的整体电化学性能. 本研究首次利用Se@C纳米棒模板, 通过原位硒化过程可控合成了一系列碳纳米管(CNT)负载的镍硒化物, 包括立方型NiSe2NiSe2/Ni0.85Se复合材料、六方型Ni0.85Se.优化后的NiSe2/Ni0.85Se/CNT复合材料具有比表面积大、孔隙率高、碳骨架空心等优点, 具有616Cg−1的高比容量、优良的倍率性能和稳定的循环寿命. 通过一系列的非原位表征和DFT计算, 深入研究了其内部的法拉第机制. 结果表明, 所制备的Ni//Zn电池在3485 W kg−1时具有311.4 W h kg−1的高能量密度和较长的循环寿命. 本研究为硒化镍基电极材料的设计提供了一种巧妙的策略, 且深入研究了其在碱性锌电池中的法拉第机理.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (21875285 and 22001265), Taishan Scholar Foundation (ts201511019), the Key Research and Development Projects of Shandong Province (2019JZZY010331), the Fundamental Research Funds for the Central Universities (19CX05001A), and the Natural Science Foundation of Shandong Province (ZR2020QB028).
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Author contributions Mei H finished the experimental section, data analysis, and original draft writing. Zhang H helped with date analysis. Li Z and Zhang L helped with characterizations and analysis. Lu X, Xu B and Sun D revised the article.
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Supplementary information Supporting data are available in the online version of the paper.
Ben Xu received his PhD degree from the Memorial University of Newfoundland in 2015. Currently, his main research interests focus on the design and synthesis of functional porous materials and their applications in the field of electrochemical energy storage.
Daofeng Sun received his PhD degree from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences in 2003. Then, he conducted his postdoctoral work at the Department of Chemistry and Biochemistry, University of Miami. He joined China University of Petroleum in 2013. His main research interests focus on the design and synthesis of crystalline porous materials, high selectivity gas adsorbents and separation membranes, and energy storage and conversion materials.
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Enabling kinetically fast activation of carbon nanotube@nickel selenide through pore-phase dual regulation in aqueous zinc battery
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Mei, H., Zhang, H., Li, Z. et al. Enabling kinetically fast activation of carbon nanotube@nickel selenide through pore-phase dual regulation in aqueous zinc battery. Sci. China Mater. 65, 929–938 (2022). https://doi.org/10.1007/s40843-021-1791-1
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DOI: https://doi.org/10.1007/s40843-021-1791-1