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Experimental and Correlative Analyses of the Ageing Mechanism of Activated Carbon Based Supercapacitor

超级电容器 活性炭 分离器(采油) 材料科学 阳极 碳纤维 化学工程 X射线光电子能谱 复合材料 化学 电极 电容 物理化学 热力学 吸附 物理 复合数 工程类
作者
Yilun Huang,Yang Zhao,Qianming Gong,Mouyi Weng,Junfei Bai,Xi Liu,Yanqi Jiang,Junjie Wang,Dazhi Wang,Yang Shao,Ming Zhao,Daming Zhuang,Ji Liang
出处
期刊:Electrochimica Acta [Elsevier BV]
卷期号:228: 214-225 被引量:50
标识
DOI:10.1016/j.electacta.2017.01.059
摘要

With the increasing needs of clean energy, supercapacitors, especially the activated carbon (AC) based supercapacitors are attracting great attentions for their theoretically infinite lifespan. However, they always age much faster than expected due to some mechanisms. In this work, we probed the ageing mechanism of AC based supercapacitors systematically by in-depth relevancy analyses of the main components in the supercapacitors after they have been aged at different temperatures for a rather long duration (1296 h) which was specially designed to simulate practical service limit of supercapacitors. On the one hand, XRD, TG-MS, XPS and BET analyses indicated that more than 23% of capacity decrease after high temperature ageing could be ascribed to the degradation of the crystal structure for the AC carbon, the agglomeration of the conductive carbon black, the collapse of the pore structure in the mixed AC layer and the separator, and the peeling off of the carbonaceous layer from the current collector, which was eroded as well during the ageing process. On the other hand, we found that the size of bare and solvated BF4− ions were about 2.86 Å and 11.11 Å, respectively, with the help of density functional theory (DFT) calculations. So the performance degradation of the supercapacitor could be ascribed to the lowered ion diffusing efficiency in the collapsed pores together with the increased electrical resistance of the whole system and the decreased specific area, which were resulted from all kinds of side-reactions ultimately. In addition, the relatively more serious ageing of the anode might be due to the more fluorochemicals and nitrogen compounds produced by side-reactions in the anodes.
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