首页> 外文期刊>Environmental Science: Nano >Accelerated Fenton-like kinetics by visible-light-driven catalysis over iron(iii) porphyrin functionalized zirconium MOF: effective promotion on the degradation of organic contaminants
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Accelerated Fenton-like kinetics by visible-light-driven catalysis over iron(iii) porphyrin functionalized zirconium MOF: effective promotion on the degradation of organic contaminants

机译:通过铁(III)卟啉官能化锆MOF的可见光催化(III)卟啉的可见光催化加速了FENTON样动力学:有效促进有机污染物的降解

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摘要

Ultraviolet (UV)-light or a cocatalyst (e.g., chelating agents) is commonly used to promote a Fenton-like technique in the treatment of organic contaminants in wastewater. However, the energy costs for generating UV and the poor recyclability of the iron (Fe)-based catalyst/cocatalyst remain primary concerns for their further implementation. Herein, we present a visible-light-driven collaborative process comprising photocatalysis and Fenton-like reaction that are both conducted using a derivative of a zirconium (Zr)-based metal-organic framework (UiO-66 MOF), in which Fe(iii) tetra(4-carboxylphenyl)porphyrin chloride (Fe-III-TCPPCl) is coordinated in the pore of UiO-66. The mixed ligand Fe-III-TCPPCl not only plays the role of a photosensitizer that fosters light absorption and suppresses the recombination of photo-induced carriers over the integrated structure, Fe-III-TCPPCl subset of UiO-66 (FTU), but also acts as a potential iron-based catalyst for decomposing hydrogen peroxide (H2O2) to engender oxidative hydroxyl radicals (OH). Furthermore, besides achieving virtually 100% decomposition of a surrogate pollutant, rhodamine B (RhB), compared with 51% achieved by photolysis alone within 60 min, introducing H2O2 into the visible-light irradiating system could also promote the mineralization of RhB, as indicated by a 15.5% increment in chemical oxygen demand (COD) removal. The photo-excited electrons partially participate in the reduction of the immobilized Fe-III-TCPPCl into Fe-II-TCPPCl, and therefore greatly accelerate the Fenton-like reaction. Moreover, the structural similarity of FTU to the robust parent UiO-66 guarantees its reliable recycling performance with respect to degradation over four times.
机译:紫外(UV) - 灯或助催化剂(例如,螯合剂)通常用于促进废水中有机污染物的芬顿状技术。然而,产生紫外线的能量成本和铁(Fe)的催化剂/助催化剂的差的可再循环性仍然是其进一步实施的主要问题。在此,我们提出了一种可见光驱动的协作方法,包括使用锆(Zr)的金属 - 有机框架(UIO-66MOF)的衍生物进行的光催化和芬顿状反应,其中Fe(III )Tetra(4-羧基苯基)卟啉氯化物(Fe-III-TCPPCL)在UIO-66的孔中配位。混合配体FeI-III-TCPCL不仅发挥光敏剂的作用,可以在荧光吸收和抑制通过综合结构上的光诱导载体的重组,FE-III-TCPPCL子集,UIO-66(FTU),而且用作分解过氧化氢(H2O2)的潜在铁基催化剂,得到氧化羟基自由基(OH)。此外,除了几乎100%分解替代污染物的分解之外,与60分钟内单独的光解相比,将H 2 O 2引入可见光照射系统中的51%,也可以促进RHB的矿化,如图所示递增15.5%的化学需氧量(COD)去除。照片激发电子部分参与将固定的Fe-III-TCPPCL的减少到Fe-II-TCPPCL中,因此极大地加速了芬顿的反应。此外,FTU对稳健父权UIO-66的结构相似性可确保其可靠的回收性能相对于四次降解。

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  • 来源
    《Environmental Science: Nano》 |2019年第8期|共10页
  • 作者单位

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Northwest Normal Univ Coll Chem &

    Chem Engn Res Ctr Gansu Mil &

    Civilian Integrat Adv Struct Lanzhou 730074 Gansu Peoples R China;

    Guangdong Univ Technol Sch Environm Sci &

    Engn Inst Environm Hlth &

    Pollut Control Guangzhou Key Lab Environm Catalysis &

    Pollut Con Guangzhou 510006 Guangdong Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 环境科学、安全科学;
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