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Chemcial Industry and Engineering 2022, Vol. 39 Issue (5) :66-77    DOI: 10.13353/j.issn.1004.9533.20220104
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Removal the oxygen-containing groups of porous carbon under low-temperature for supercapacitors
YANG Ting1, YIN Likun2, HAN Yu2, BI Ran2, ZHENG Zhuangzhuang1, ZHANG Yanan1, CHEN Mingming1
1. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. Comprehensive Energy Research Center, Institute of Science and Technology, China Three Gorges Corporation, Beijing 100038, China

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Abstract The key to increasing the energy density of electric double-layer capacitors (EDLCs) is to widen the voltage window of EDLCs and improve the withstanding voltage characteristics of porous carbon electrode materials. However, the current difficulty in improving the withstanding voltage characteristics of porous carbon is to reduce the content of oxygen-containing functional groups without destroying the hierarchical pore structure. In this paper, by using a nickel-based catalyst, the hydrogen spillover phenomenon on the surface of the catalyst was applied to remove the oxygen-containing groups of the porous carbon under low temperature conditions, thereby obtaining a porous carbon with low oxygen content. Compared with thermal reduction (H2 atmosphere), in addition to pyrolysis and hydrogenation reactions, the reduction process under hydrogen spillover also includes violent hydrogenation reactions involving highly active hydrogen atoms. Besides, the mechanisms of removing oxygen-containing groups under the primary hydrogen spillover and second hydrogen spillover are investigated and compared in detail. Under the primary hydrogen spillover, due to the strong chemical interaction (Ni—O—C bond and Ni—C bond) between the nickel nanoparticles and the porous carbon, the removal of oxygen-containing groups in the porous carbon is inhibited. However, under the second hydrogen spillover, the Ni—C bond and Ni—O—C bond are avoided, and the dissociated highly active hydrogen atoms diffuse for a long distance at the centimeter level, which can more effectively remove C—O and CO groups. In addition, under the second hydrogen spillover, the crystallinity of carbon layer structure in obtained porous carbon PC-Ni-655 is improved and the pore structure is not destroyed. As a result, when PC-Ni-655 was applied as the electrode material of EDLCs, a small self-discharge phenomenon and long-term cycling stability (a capacity retention rate is 87.9% over 5 000 cycles at 1 A·g-1) with a high operation voltage of 3.3 V were obtained.
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YANG Ting
YIN Likun
HAN Yu
BI Ran
ZHENG Zhuangzhuang
ZHANG Yanan
CHEN Mingming
Keywordssupercapacitors   oxygen-containing functional groups   hydrogen spillover   porous carbon   withstanding voltage characteristics   electrochemical performance     
Received 2022-01-08;
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YANG Ting, YIN Likun, HAN Yu, BI Ran, ZHENG Zhuangzhuang, ZHANG Yanan, CHEN Mingming.Removal the oxygen-containing groups of porous carbon under low-temperature for supercapacitors[J]  Chemcial Industry and Engineering, 2022,V39(5): 66-77
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