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首页> 外文期刊>Environmental Science & Technology >Probing the Surface Reactivity of Pyrogenic Carbonaceous Material (PCM) through Synthesis of PCM-Like Conjugated Microporous Polymers
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Probing the Surface Reactivity of Pyrogenic Carbonaceous Material (PCM) through Synthesis of PCM-Like Conjugated Microporous Polymers

机译：通过合成类似PCM的共轭微孔聚合物来探索热解碳质材料（PCM）的表面反应性

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摘要

Pyrogenic carbonaceous matter (PCM) is redoxactive and promotes both abiotic and biotic reactions in the environment, possibly as a result of its conductivity and phenolic/quinone functional groups. However, due to the complexity of PCM, the contribution of conductivity or phenolic/quinone functional groups to its redox activity is poorly understood, which hinders its potential engineering applications. Here, we synthesized tunable conjugated microporous polymers (CMPs) that possess key properties of PCM, which can be used as PCM analogues to provide insights to PCM reactivity. Specifically, controlled incorporation of phenolic moieties into CMPs during polymer synthesis affected electron-donating capacity, while carbonization of CMPs at various temperatures altered conductivity. Both properties were then correlated with PCM reactivity measured by the decay kinetics of a model pollutant trichloronitromethane. We demonstrate that some of the prepared CMPs enabled transformation of trichloronitromethane, while no decay was observed in the absence of CMPs. Results of further investigation suggest that trichloronitromethane decay occurs by reductive dechlorination, suggesting that CMPs are electron donors and the first dissociative electron transfer from CMPs was likely to be the rate-limiting step. Conductivity but not electron-donating capacity was positively correlated with CMP-mediated trichloronitromethane decay kinetics, suggesting an important role of the electron transfer kinetics at the interface for PCM-mediated transformation of environmental pollutants.
机译：热解碳质物质（PCM）具有氧化还原活性，并可能在环境中促进非生物和生物反应，这可能是由于其导电性和酚/醌官能团所致。然而，由于PCM的复杂性，人们对导电性或酚/醌官能团对其氧化还原活性的贡献了解甚少，这阻碍了其潜在的工程应用。在这里，我们合成了具有PCM关键特性的可调共轭微孔聚合物（CMP），可用作PCM类似物以提供PCM反应性的见解。具体而言，在聚合物合成过程中，将酚类部分掺入CMP中会影响供电子能力，而CMP在各种温度下的碳化都会改变电导率。然后将这两个特性与通过模型污染物三氯硝基甲烷的衰减动力学测量的PCM反应性相关。我们证明了一些制备的CMP使三氯硝基甲烷转化，而在没有CMP的情况下未观察到衰变。进一步研究的结果表明，三氯硝基甲烷的降解是通过还原性脱氯而发生的，这表明CMP是电子给体，从CMP进行的第一个解离电子转移很可能是限速步骤。电导率而不是电子给体容量与CMP介导的三氯硝基甲烷衰变动力学呈正相关，表明电子转移动力学在PCM介导的环境污染物转化中的重要作用。

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  • 来源
    《Environmental Science & Technology》 |2019年第13期|7673-7682|共10页
  • 作者

    Li Zhao; Mao Jingdong; Chu Wenying; Xu Wenqing;

  • 作者单位

    Villanova Univ, Dept Civil & Environm Engn, Villanova, PA 19085 USA;

    Old Dominion Univ, Dept Chem & Biochem, Norfolk, VA 23529 USA;

    Old Dominion Univ, Dept Chem & Biochem, Norfolk, VA 23529 USA;

    Villanova Univ, Dept Civil & Environm Engn, Villanova, PA 19085 USA;

  • 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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