Selective Heterogeneous Fenton Degradation of Formaldehyde Using the Fe-ZSM-5 Catalyst
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PROVIDER: S-EPMC11206745 | biostudies-literature | 2024 Jun
REPOSITORIES: biostudies-literature
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Project description:In this study, the Fe-containing tailings (Fe-TO) ore was reutilized and enriched with FeCl3 as a heterogeneous catalyst for the Fenton process to degrade the organic dyes from aqueous solution. The determinants of the heterogeneous catalytic Fenton system which included iron modification ratio, solution pH, catalyst dosage, H2O2 dosage and initial concentration of organic dyes were systematically investigated. The modification ratio of 15% (w/w of iron), pH of 3, MFe-TO15 dosage of 0.5 g L-1 and H2O2 dosage of 840 mg L-1 were chosen as the best operational conditions for Fenton oxidation of organic dyes. The decolorization efficiency of both MB and RhB by MFe-TO15/H2O2 was higher than that of Fe-TO/H2O2 by about two times. The kinetic study showed the degradation of organic dyes well fitted the pseudo-first-order kinetic model with apparent constant rate values (K d) following the same sequence as the degradation efficiency of organic dyes. The degradation mechanism of dyes could be attributed to adsorption due to the good-development in textural properties of the iron modified catalyst (MFe-TO) with an increase in BET surface area, pore volume and pore diameter of, respectively, 2, 5 and 5 times and leaching iron through homogeneous Fenton reaction. However, the oxidation process occurring on the MFe-TO15's surface by heterogeneous Fenton reaction which enhanced decomposition of H2O2 for continuous generation of hydroxyl radicals was the main mechanism. The key role of *OH radical in oxidation of organic dyes was further ascertained by the remarkable drop in the decolorization of both organic dyes when the various radical-scavengers, including tert-butanol and chloride were supplemented into Fenton systems. A good stability of the catalyst was obtained through leaching test with low leaching iron ratio. The applied modified catalyst remained stable through three consecutive runs. From these findings, it can be concluded that the modified material can be applied as a feasible, inexpensive and highly effective catalyst for removal of persistent organic compounds from wastewater.
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Project description:The selective oxidation of CH4 in the aqueous phase to produce valuable chemicals has attracted considerable attention due to its mild reaction conditions and simple process. As the most widely studied catalyst for this reaction, Fe-ZSM-5 demonstrates high intrinsic activity and selectivity; however, Fe-ZSM-5 prepared using conventional methods has a limited number of active Fe sites, resulting in low CH4 conversion per unit mass of the catalyst. This study reports a facile organic-template-free synthesis strategy that enables the incorporation of more Fe into the zeolite framework with a higher dispersion degree compared to conventional synthesis methods. Because framework Fe incorporated in this way is more readily transformed into isolated extra-framework Fe species under thermal treatment, the overall effect is that Fe-ZSM-5 prepared using this method (Fe-HZ5-TF) has 3 times as many catalytically active sites as conventional Fe-ZSM-5. When used for the selective oxidation of CH4 with 0.5 M H2O2 at 75 °C, Fe-HZ5-TF produced a high C1 oxygenate yield of 109.4 mmol gcat-1 h-1 (a HCOOH selectivity of 91.1%), surpassing other catalysts reported to date. Spectroscopic characterization and density functional theory calculations revealed that the active sites in Fe-HZ5-TF are mononuclear Fe species in the form of [(H2O)3Fe(IV)═O]2+ bound to Al pairs in the zeolite framework. This differs from conventional Fe-ZSM-5, where binuclear Fe acts as the active site. Analysis of the catalyst and product evolution during the reaction suggests a radical-driven pathway to explain CH4 activation at the mononuclear Fe site and subsequent conversion to C1 oxygenates.
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