Catalytic oxidation of organic pollutants on pristine and surface nitrogen-modified carbon nanotubes with sulfate radicals

Catalytic oxidation of organic pollutants on pristine and surface nitrogen-modified carbon nanotubes with sulfate radicals
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DOI:
10.1016/j.apcatb.2014.02.012
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发表时间:
2014-07-01
影响因子:
22.1
通讯作者:
Wang, Shaobin
Wang, Shaobin
中科院分区:
化学1区
文献类型:
--
作者:
Sun, Hongqi;Kwan, ChungKeat;Wang, Shaobin

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利用无金属纳米碳或碳质材料作为环境水体修复的催化剂是一种很有前途的清洁方法,因为绿色碳材料可以完全防止潜在的有毒金属浸出和对水体的二次污染。本研究报告,原始多壁碳纳米管(MWCNTs)可以有效地激活过一硫酸盐(PMS)和过二硫酸盐(或过硫酸盐,过二硫酸盐,PDS),产生硫酸根自由基氧化苯酚溶液。采用硝酸铵低温退火法对碳纳米管进行表面氮改性,并对氮改性碳纳米管(N-CNT)进行了表征。结果表明,碳纳米管表面氮改性对PMS和PDS的活化效果不同。N-CNT能显著提高PMS对苯酚的降解率,但降低PDS对苯酚的降解率。讨论了碳纳米管基材料催化硫酸根氧化苯酚溶液的反应动力学和机理。(C)2014爱思唯尔有限公司版权所有。
Employing metal-free nanocarbons or carbonaceous materials as a catalyst for environmental water remediation is a promising clean approach because the green carbon materials can completely prevent the potential toxic metal leaching and secondary contamination to water body. This study reports that pristine multi-walled carbon nanotubes (MWCNTs) can effectively activate peroxymonosulfate (PMS) and peroxydisulfate (or persulfate, perdisulfate, PDS) to produce sulfate radicals for oxidation of phenol solutions. Surface nitrogen modification was conducted by a facile synthesis via annealing MWCNTs with ammonium nitrate at a low temperature and the nitrogen modified MWCNTs (N-CNT) was characterized by a variety of techniques. It was found that surface nitrogen modification of MWCNTs produced different effects on PMS and PDS activation. N-CNT can significantly improve the phenol degradation with PMS, but decrease the degradation efficiency with PDS. Reaction kinetics and the mechanism in catalytic oxidation of phenol solutions with sulfate radicals over CNT-based materials were discussed. (C) 2014 Elsevier B.V. All rights reserved.