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用于超快锌离子混合超级电容器的三维分级多孔碳阴极中氮和氧掺杂剂的协同效应

Synergistic effect of nitrogen and oxygen dopants in 3D hierarchical porous carbon cathodes for ultra-fast zinc ion hybrid supercapacitors.

作者信息

Wen Fuwang, Yan Yuan, Sun Shirong, Li Xu, He Xing, Meng Qingwei, Zhe Liu Jefferson, Qiu Xueqing, Zhang Wenli

机构信息

Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology (GDUT), 100 Waihuan Xi Road, Panyu District, Guangzhou 510006, China.

Department of Mechanical Engineering, The University of Melbourne, Parkville, VIC 3010, Australia.

出版信息

J Colloid Interface Sci. 2023 Jun 15;640:1029-1039. doi: 10.1016/j.jcis.2023.03.024. Epub 2023 Mar 8.

Abstract

Zinc-ion hybrid supercapacitor is one of the most promising electrochemical energy storage devices for the applications needing both high energy densities and power densities. Nitrogen doping is an effective way to enhance the capacitive performance of porous carbon cathodes in zinc-ion hybrid supercapacitor. However, accurate evidence is yet needed to demonstrate how nitrogen dopants influence the charge storage of Zn and H cations. Herein, we prepared 3D interconnected hierarchical porous carbon nanosheets by a one-step explosion method. The effect of nitrogen dopants on pseudocapacitance was analyzed by the electrochemical behaviors of as-prepared porous carbon samples with similar morphology and pore structure but different nitrogen and oxygen doping levels. Ex-situ XPS and DFT calculation demonstrate that nitrogen dopants promote the pseudocapacitive reactions by lowering the energy barrier for the change of oxidation states of carbonyl moieties. Owing to the improved pseudocapacitance by nitrogen/oxygen dopants and fast diffusion of Zn ions in 3D interconnected hierarchical porous carbon matrix, the as-constructed ZIHCs show both high gravimetric capacitance (301 F g at 0.1 A g) and excellent rate capability (a capacitance retention of 30% at 200 A g).

摘要

锌离子混合超级电容器是最具前景的电化学储能装置之一,适用于需要高能量密度和功率密度的应用场景。氮掺杂是提高锌离子混合超级电容器中多孔碳阴极电容性能的有效方法。然而,仍需要准确的证据来证明氮掺杂剂如何影响锌和氢离子的电荷存储。在此,我们通过一步爆炸法制备了三维互连的分级多孔碳纳米片。通过对具有相似形态和孔结构但氮和氧掺杂水平不同的多孔碳样品的电化学行为分析,研究氮掺杂剂对赝电容的影响。非原位XPS和DFT计算表明,氮掺杂剂通过降低羰基部分氧化态变化的能垒来促进赝电容反应。由于氮/氧掺杂剂提高了赝电容,以及锌离子在三维互连分级多孔碳基质中的快速扩散,所构建的锌离子混合超级电容器表现出高的质量比电容(在0.1 A g时为301 F g)和优异的倍率性能(在200 A g时电容保持率为30%)。

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