DEVELOPMENT OF A NEW HETEROGENEOUS CATALYST FOR THE USE IN FENTON-LIKE PROCESS TOWARD THE REMOVAL OF PESTICIDES FROM WATER

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2022-8-31

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Ali, Mohsin

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With the primary aim of developing a new heterogeneous catalyst from natural zeolite chabazite (CHA) for use in Fenton-like process, the removal of malathion (MLT) and carbendazim (CBD) pesticides from water were investigated. To improve the physicochemical properties of natural CHA, different pretreatment techniques, namely, NH4+-exchange, steam treatment (dealumination), and acid/alkali treatment (desilication), were applied. CHA samples were characterized by XRD, N2 adsorption, UV-Vis, SEM-EDX, ICP, and NMR to monitor the improvement after each pretreatment step. The steam treatment was superior to the desilication, improving the mesopore volume from 0.036 to 0.070 cm3/g when operated at 675 oC and 20 kPa. This increase in mesopore volume enabled Fe3+ to increase from 0.24 to 0.60 mmol Fe3+/g CHA following the Fe-exchange. The pretreated and Fe-exchanged CHA (Fe-CHA) was used for pesticide oxidation, and the effect of H2O2, pH, catalyst dose, and pesticide concentration were investigated using Box-Behnken Design. Results revealed that Fenton-like oxidation could work at a higher and wider pH range (pH 3-7) compared to classical Fenton. The highest MLT and CBD removal efficiencies were attained as 81 and 88%, respectively, when H2O2, Fe-CHA, and pH parameters were set as 150 mg/L, 750 mg/L, and 5, respectively. Additionally, the performance of Fe-CHA was compared with commercially available synthetic zeolites Fe-USY and Fe-ZSM-5. To understand the pesticide removal mechanism, oxidation and adsorption kinetic studies were carried out. The reusability study showed that Fe-CHA could be used several times (at least 5 times) after regeneration, and sludge production was 25-40 times lower than classical Fenton. Effect of water matrix on MLT and CBD removal was also sought. Moreover, by-product analyses for both pesticides were performed. Though by-products of CBD could not be determined, malaoxon, desmethyl malaoxon, and diethyl malate were identified as by-products of MLT degradation. Accordingly, a possible oxidation pathway for MLT was proposed.

Subject Keywords

Fe-Chabazite, Fenton-like Oxidation, Heterogeneous Catalysts, Malathion, Carbendazim

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https://hdl.handle.net/11511/99452

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Graduate School of Natural and Applied Sciences, Thesis

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Citation Formats

M. Ali, “DEVELOPMENT OF A NEW HETEROGENEOUS CATALYST FOR THE USE IN FENTON-LIKE PROCESS TOWARD THE REMOVAL OF PESTICIDES FROM WATER,” Ph.D. - Doctoral Program, Middle East Technical University, 2022.