Cu2O@β-cyclodextrin as a synergistic catalyst for hydroxyl radical generation and molecular recognitive destruction of aromatic pollutants at neutral pH.
Cu2O@β-cyclodextrin as a synergistic catalyst for hydroxyl radical generation and molecular recognitive destruction of aromatic pollutants at neutral pH.
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DOI：
10.1016/j.jhazmat.2018.05.065
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发表时间：
2018-09
影响因子：
13.6
通讯作者：
Lingshuai Kong;Guodong Fang;Yanyun Kong;Meng Xie;V. Natarajan;Dong-mei Zhou;J. Zhan
中科院分区：
文献类型：
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作者：
Lingshuai Kong;Guodong Fang;Yanyun Kong;Meng Xie;V. Natarajan;Dong-mei Zhou;J. Zhan
废水系统含有大量的化合物，如人为芳香族污染物和天然有机物（NOM），并且通常具有高于4的pH值。类Fenton反应是去除有机污染物最常用的方法，但由于羟基自由基和螯合剂的竞争作用，NOM会抑制有机污染物与H2 O2的反应活性。本工作以Cu2O @ β-CD为载体，在中性pH条件下实现了分子识别与类Fenton催化的协同作用，从而实现了对芳香族污染物的降解。β-CD的交联可以有效地抑制腐殖酸对Cu 2 O表面催化性能的干扰，抑制Cu的浸出。结果表明，在中性pH条件下，Cu2O@β-CD的催化活性（0.0331 min−1）高于Cu 2 O（0.0064 min−1），并提出了Cu2O@β-CD/BPA/H2 O2体系中Cu+、β-CD和苯氧-Cu 2+配合物协同催化的机理.将分子识别耦合到类Fenton反应中的策略为在中性pH下降解芳香族污染物提供了一种有效的途径。
Wastewater systems contain a large number of compounds, such as anthropogenic aromatic pollutants and natural organic matter (NOM), and usually have pH higher than 4. Fenton-like reaction is the most widespread method for removal of organic pollutants, but their reactivity with H2O2may be inhibited by NOM due to the competition of hydroxyl radicals and chelating agents. In this work, Cu2O@β-cyclodextrin was developed to achieve the collaboration between molecular recognition and Fenton-like catalysis to destruct aromatic pollutants at neutral pH. In Cu2O@β-CD, covalent Cusingle bondOsingle bondC bond was topotaxially converted from CuCl assisted by β-CD at room temperature. Covalently linked β-CD could keep humic acid from interfering catalytic performance of Cu2O surfaces and inhibit the leaching of copper. A higher catalytic ability was observed for Cu2O@β-CD with rate constant 0.0331 min−1than Cu2O (0.0064 min−1) at neutral pH. A mechanism of synergistic catalysis was proposed on the basis of Cu+, β-CD and phenoxo-Cu2+complexes in the Cu2O@β-CD/BPA/H2O2system. The strategy of coupling molecular recognition into Fenton-like reaction provides an efficient and promising approach to the destruction of aromatic pollutants at neutral pH.