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首页> 外文期刊>Environmental Science & Technology >Catalytic Effects of Functionalized Carbon Nanotubes on Dehydrochlorination of 1,1,2,2-Tetrachloroethane
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Catalytic Effects of Functionalized Carbon Nanotubes on Dehydrochlorination of 1,1,2,2-Tetrachloroethane

机译:功能化碳纳米管对1,1,2,2-四氯乙烷脱氯化氢的催化作用

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摘要

The environmental implications of carbon nanomaterials have received much attention. Nonetheless, little is known about how carbon nanomaterials might affect the abiotic transformation of organic contaminants in aquatic environments. In this study, we observed that three functionalized multiwalled carbon nanotubes (MWCNTs)-including a hydroxylated MWCNT (OH-MWCNT), a carboxylated MWCNT (COOH-MWCNT), and an aminated MWCNT (NH_2-MWCNT)-all had strong catalytic effects on the dehydrochlorination of 1,1,2,2-tetrachloroethane (TeCA) at three different pH (7, 8, and 9); notably, the most significant effects (up to 130% increase in reaction rate) were observed at pH 7, at which reaction kinetics was very slow in the absence of MWCNT. The primary mechanism was that the -NH_2 group and the deprotonated -COOH and -OH groups serve as bases to catalyze the reaction. Modeling results indicate that at any given pH the transformation kinetic constants of MWCNT-adsorbed TeCA were up to 2 orders of magnitude greater than the respective kinetic constant of dissolved TeCA. The overall catalytic effects of the MWCNTs depended both on the basicity of the surface functionalities of MWCNT and on the adsorption affinities of MWCNT for TeCA. Interestingly, Suwannee River humic acid-selected as a model dissolved organic matter-had negligible effects on the dehydrochlorination kinetics, even though it is rich in surface O-runctionalities. An important environmental implication is that carbon nanotubes released into the environment might significantly affect the fate of chlorinated solvents.
机译:碳纳米材料对环境的影响已引起广泛关注。但是,对于碳纳米材料如何影响水生环境中有机污染物的非生物转化知之甚少。在这项研究中,我们观察到三个功能化的多壁碳纳米管(MWCNT),包括羟基化的MWCNT(OH-MWCNT),羧化的MWCNT(COOH-MWCNT)和胺化的MWCNT(NH_2-MWCNT),均具有较强的催化作用。 1,3,2-三氯乙烷(TeCA)在三种不同pH(7、8和9)下的脱氯化氢反应;值得注意的是,在pH值为7时,观察到了最显着的效果(反应速率提高了130%),在没有MWCNT的情况下,反应动力学非常缓慢。其主要机理是-NH_2基团和去质子化的-COOH和-OH基团是催化反应的碱。建模结果表明,在任何给定的pH值下,MWCNT吸附的TeCA的转化动力学常数都比溶解的TeCA的相应动力学常数高2个数量级。 MWCNT的总体催化作用取决于MWCNT的表面官能度的碱性和取决于MWCNT对TeCA的吸附亲和力。有趣的是,尽管Suwannee River腐殖酸富含表面O型成分,但它对脱氢动力学的影响却可以忽略不计,它被选为溶解有机物的模型。一个重要的环境影响是释放到环境中的碳纳米管可能会严重影响氯化溶剂的命运。

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  • 来源
    《Environmental Science & Technology》 |2014年第7期|3856-3863|共8页
  • 作者单位

    College of Environmental Science and Engineering/Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Nankai University, Tianjin 300071, China;

    State Key Laboratory of Pollution Control and Resource Reuse/School of the Environment, Nanjing University, Nanjing, Jiangsu 210093, China;

    State Key Laboratory of Pollution Control and Resource Reuse/School of the Environment, Nanjing University, Nanjing, Jiangsu 210093, China;

    College of Environmental Science and Engineering/Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Nankai University, Tianjin 300071, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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