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Enhancing the Fenton-like Catalytic Activity of nFe_2O_3 by MIL-53(Cu) Support: A Mechanistic Investigation

机译:MIL-53(Cu)载体增强nFe_2O_3 Fenton类催化活性的机理研究

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摘要

A novel Fenton-like catalyst was synthesized by immobilizing nano-Fe_2O_3 (nFe_2O_3) on MIL-53(Cu). The pseudo-first-order rate constant of bisphenol A degradation in the nFe_2O_3/MIL-53(Cu)/H_2O_2 system reached 0.0123 min~(-1), while the values in MIL-53(Cu)/H_2O_2 and nFe_2O_3/H_2O_2 systems were only 0.0026 and 0.0040 min~(-1), respectively. The characterization of nFe_2O_3/MIL-53(Cu) reveals that the supreme catalytic activity of this material could be ascribed to iron—copper synergy, smaller size, and better dispersion of nFe_2O_3 particles. Moreover, a method of trapping Cu(I) by neocuproine was developed, which could shield Cu(I) from interacting with iron and H_2O_2, and thus allow quantitative differentiation of the contribution to the enhanced catalytic activity by each of the factors. Using this method, 19% of the enhancement was determined to be contributed by synergistic effect, while 24% of the enhancement was due to the smaller size and better dispersion of the nFe_2O_3, particles on MIL-53(Cu) support. In addition, the performance of nFe_2O_3/MIL-53(Cu) only dropped 10.7% after five treatment cycles in real wastewater, showing good potential in practical application. We believe this study sheds light on the tailored design of Fenton-like catalysts and elucidates the catalytic mechanisms of supported bimetallic catalysts.
机译:通过将纳米Fe_2O_3(nFe_2O_3)固定在MIL-53(Cu)上合成了一种新型的Fenton类催化剂。 nFe_2O_3 / MIL-53(Cu)/ H_2O_2系统中双酚A降解的拟一级反应速率常数达到0.0123 min〜(-1),而MIL-53(Cu)/ H_2O_2和nFe_2O_3 / H_2O_2中的双酚A降解速率为准一级。系统分别只有0.0026和0.0040 min〜(-1)。 nFe_2O_3 / MIL-53(Cu)的表征表明,该材料的最高催化活性可归因于铁-铜协同作用,较小的尺寸以及nFe_2O_3颗粒的较好分散性。此外,开发了一种新铜环丙氨酸捕获铜(I)的方法,该方法可以屏蔽铜(I)与铁和H_2O_2的相互作用,从而可以定量区分每种因素对增强催化活性的贡献。使用这种方法,确定了19%的增强作用是由协同效应贡献的,而24%的增强作用是由于较小的尺寸和更好的nFe_2O_3颗粒在MIL-53(Cu)载体上的分散。此外,在实际废水中经过五个处理周期后,nFe_2O_3 / MIL-53(Cu)的性能仅下降了10.7%,在实际应用中显示出良好的潜力。我们相信这项研究为Fenton类催化剂的定制设计提供了启示,并阐明了负载型双金属催化剂的催化机理。

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  • 来源
    《Environmental Science & Technology》 |2020年第8期|5258-5267|共10页
  • 作者单位

    State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing 210023 China;

    State Key Laboratory of Pollution Control and Resource Reuse School of the Environment and Research Center for Environmental Nanotechnology (ReCENT) Nanjing University Nanjing 210023 China;

    Environmental Engineering and Science Program Department of Chemical and Environmental Engineering University of Cincinnati Cincinnati Ohio 45221-0012 United States;

    Department of Environmental Science and Engineering Nanjing Agricultural University Nanjing 210095 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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