Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis

Unzipping carbon nanotubes to nanoribbons for revealing the mechanism of nonradical oxidation by carbocatalysis
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将碳纳米管解压缩为纳米带,揭示碳催化非自由基氧化机制

DOI:
10.1016/j.apcatb.2020.119146
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发表时间:
2020-11
期刊:
Applied Catalysis B: Environmental
影响因子:
--
通讯作者:
Shaobin Wang
Shaobin Wang
中科院分区:
其他
文献类型:
--
作者:
Qi Yang;Yidi Chen;Xiaoguang Duan;Shanke Zhou;Yue Niu;Hongqi Sun;Linjie Zhi;Shaobin Wang

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石墨多壁碳纳米管(MWCNTs)可控地解压缩成边缘丰富的石墨烯纳米带,以揭示边缘和缺陷在过硫酸盐活化双酚A(BPA)氧化中的作用。富集的碳边缘显著提高催化性能,并且可以作为杂原子(N,S)掺杂的宿主位点来促进碳催化。样品(NS-2)在20分钟内完全去除BPA,速率常数为0.182 min-1。速率常数与缺陷形态形成有关,与拉曼光谱的指示剂(ID/ID ')呈负相关。过多的边缘导致缺陷和sp2到sp3的结构转变,导致有机氧化的恶化。此外,通过自由基筛选试验、原位拉曼和电化学表征,证实了未压缩的多壁碳纳米管遵循非自由基电子转移途径。揭示的机理强调了在边缘富集碳催化剂中必要的石墨化度和导电性对于更好的催化性能的重要性。
Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min-1. The rate constants were relating to the defect speciation in a negative correlation to an indicator (ID/ID’) from Raman spectra. Excessive edges induce defects and structure transformation of sp2to sp3, resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.
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