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The Heterogeneousfenton Reaction System Applied For The Remediation Of Low-level Organic Compounds In Water:Catalyst Design And Mechanistic Study

Posted on:2015-02-15Degree:DoctorType:Dissertation
Country:ChinaCandidate:X J YangFull Text:PDF
GTID:1261330428475608Subject:Chemical Engineering
Abstract/Summary:PDF Full Text Request
The development of solid Fenton-like catalysts and its application on the remediation of low-level organic compounds in water have been studied. With the combination of the new study strategy and experimental methods, the structure of the catalysts and its relationship with the performance on the remedy of wastewater were established. FeOCl with layer structure and the supported Au/C catalyst were prepared and used for the creation of hydroxyl radicals (HO) by the decomposition of hydrogen peroxide (H2O2).Various persistent organic compounds, which usually contaminated surface water even at ppm levels, was degraded in the developed Fenton-like FeOCl systems. Most of compounds can be degraded completely within30min. The HO-radicals were attributed to the Fenton activity, being verified by the DMPO-trapped EPR spectrum and themolecular probe methodThe generation rate of HO-over FeOCl was evaluated to be1-3orders of magnitude higher than that over other solid iron-containing minerals. Moreover, by a melt-infiltration method, the preparation route of supported FeOCl-based Fenton-like catalyst was prepared in a large scale. A kinetic modeling was built in the case of FeOCl/SiO2. The surface reaction rather than the diffusion process was dominated the decomposition process of H2O2. While the generation of HO-was demonstrated to be controlled by the decay of active complex formatted by FeOCl and H2O2.Moreover, a Au/C catalyst was also prepared and showed high HO-generation efficiency. Over a styrene-based activated carbon, uniformAu nanoparticles (NPs) wasdeposited by a modified ion-exchange method. The catalyst exhibited excellent activity for the Fenton degradation of bisphenol A. The affection of key factors, such as initial pH, reaction temperature, the loading amount of H2O2on the degradation of BPA and the decay of H2O2, were studied systematically. The structure-performance relationship of the catalyst was investigated by various techniques.The decay pathway was converted from double electron process to single electron process. The process of H2O2was further described by a set of elemental reaction network, namely a dual intermediates mechanism.
Keywords/Search Tags:Heterogeneous Fenton, H2O2decomposition, Hydroxyl radical, FeOCl, nano Au, Au-C interaction
PDF Full Text Request
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