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    Diclofenac removal by pyrite-Fenton process: Performance in batch and fixed-bed continuous flow systems
    (Elsevier Science Bv, 2019) Oral, Ozlem; Kantar, Cetin
    This study provides experimental results from batch and column studies to investigate diclofenac degradation by pyrite-Fenton process under variable chemical conditions (e.g., pyrite loading). Batch experiments show that diclofenac removal increased with increasing hydrogen peroxide and pyrite concentration. On the other hand, the addition of organic chelating agents such as citrate had an adverse effect on diclofenac removal by pyrite-Fenton process in batch systems due to scavenging effect of these agents for hydroxyl radicals. Batch results showed a direct correlation between the rate of diclofenac degradation and the rate of iron dissolution from pyrite, suggesting that diclofenac removal by pyrite-Fenton process was mainly controlled by solution phase hydroxyl radical attack on aromatic structure. Column experiments show that the effluent diclofenac concentration initially reached a peak value, and then sharply decreased to zero at higher pore volumes. The initial diclofenac breakthrough coincided well with the highest Fe(II) concentration observed in the breakthrough curve, implying that the generation of excess Fe(II) had a detrimental effect on removal efficiency due to scavenging effect of excess Fe(II) for hydroxyl radicals. The column system continued to function with 100% diclofenac removal efficiency when the effluent Fe(II) concentration decreased to a level at which the scavenging effect was minimized. (C) 2019 Elsevier B.V. All rights reserved.
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    Effect of organic ligands on oxidative degradation of chlorophenolic compounds (CP) with modified-Fenton process using pyrite as the catalyst
    (Amer Chemical Soc, 2018) Kantar, Cetin; Oral, Ozlem; Oz, Nilgun
    [Anstract Not Available]
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    Effect of pyrite on the treatment of chlorophenolic compounds with zero-valent iron-Fenton process under uncontrolled pH conditions: reaction mechanism and biodegradability
    (Springer, 2024) Oral, Ozlem; Kantar, Cetin; Yildiz, Ilker
    This current study explored the effect of pyrite on the treatment of chlorophenolic compounds (CP) by Fenton process with micron-sized zero-valent iron (ZVI) as the catalyst. The experiments were conducted in batch reactors with 100 mg L?1 CP, 0–0.02 M H2O2, and variable pyrite and ZVI doses (0–1 g L?1). Our findings show that while the reactor with 1 g L?1 ZVI as the only catalyst achieved only 10% CP removal efficiency due to rapid ZVI surface passivation and ZVI particle aggregation, the CP removal efficiency increased with increasing pyrite dose and reached 100% within couple of minutes in reactors with 0.8 g L?1 pyrite and 0.2 g L?1 ZVI. The CP removal was mainly driven by the oxidative treatment of CPs with some strong radicals such as hydroxyl radicals (•OH) while the adsorption onto the catalyst surface was only responsible for 10 to 25% of CP removals, depending on the type of CP studied. The positive impact of pyrite on CP removal by the ZVI/H2O2 system could be attributed to the ability of pyrite to (1) create an acidic environment for optimum Fenton process, (2) provide support material for ZVI to minimize ZVI particle agglomeration, and (3) stimulate iron redox cycling for improved surface site generation. Following oxidative Fenton treatment, the degradation intermediate products of CPs, including some aromatic compounds (benzoquinone, hydroquinone, etc.) and organic acids (e.g., acetic acid), became more biodegradable in comparison to their mother compounds. Overall, the treatment systems with a mixture of ZVI and pyrite as catalyst materials could offer a suitable cost-effective technology for the treatment of wastewater containing biologically non- or low-degradable toxic compounds such as chlorophenols. © The Author(s) 2024.
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    Ligand enhanced pharmaceutical wastewater treatment with Fenton process using pyrite as the catalyst: Column experiments
    (Pergamon-Elsevier Science Ltd, 2019) Kantar, Cetin; Oral, Ozlem; Oz, Nilgun Ayman
    Advanced oxidation processes offer practical and cost effective solutions for the treatment of poorly biodegradable industrial wastewaters. Here, column experiments were performed to understand the role of a complexing agent, citrate, on Fenton-treatment of an actual pharmaceutical wastewater with pyrite as the catalyst under dynamic flow conditions. Our results suggest that the pharmaceutical wastewater treatment with Fenton reaction using pyrite as the catalyst was mainly regulated by the extent of Fe dissolution from pyrite, which, in turn, resulted in formation of hydroxyl radicals in solution. The Fenton treatment efficiency was much lower in the absence of citrate compared to citric acid containing systems due to clogging of column pores with oxidized Fe species. On the other hand, the addition of citrate to wastewater significantly improved Fenton process efficacy, and prolonged the lifecycle of pyrite-packed columns depending on solution pH. Low pH values were favorable for better Fenton efficiency in systems containing citrate due to combined effect of proton and ligand promoted dissolution and mobilization of oxidized Fe species. (C) 2019 Elsevier Ltd. All rights reserved.
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    Methylene blue treatment with zero-valent iron/pyrite/H2O2 system under static and continuous flow conditions: Reaction mechanism and toxicity evaluation
    (Elsevier Science Inc, 2024) Oral, Ozlem; Arslan, Sevki; Dogan, Nazime Mercan; Yildiz, Ilker; Kantar, Cetin; Abdelsalam, Amine Hafis; Kuzucu, Volkan
    Laboratory batch and continuous flow studies, coupled with surface and toxicity analysis, were performed to evaluate methylene blue treatment by heterogeneous Fenton process using zero-valent iron (ZVI) and pyrite as co-catalyst. The use of pyrite in batch reactors significantly enhanced methylene blue treatment by the ZVI/H2O2 system because of improved iron redox cycling. The continuous-flow experiments revealed that the reactor performance increased in the order of: ZVI/H2O2 < pyrite/H2O2 < ZVI/pyrite/H2O2 under dynamic flow conditions. The methylene blue treatment by the ternary ZVI/pyrite/H2O2 system was described by an initial degradation of methylene blue with *OH radicals, followed by the adsorption and/or co-precipitation of degradation intermediates with some spherical particles. The surface analysis showed that these spherical particles formed, even at pH less than 4. The genotoxicity and cytotoxicity tests performed on mouse embryonic fibroblast (3 T3-L1) and human embryonic kidney (HEK293) cell lines showed that the Fenton treatment of methylene blue using the ZVI/pyrite/H2O2 system resulted in the formation of degradation species with much lower toxicity levels relative to methylene blue. Moreover, the Fenton degradation species of methylene blue significantly enhanced the metabolic activity of several bacterial strains, including E. coli ATCC 8739 and P. aeruginosa PAO1.
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    Oxidative degradation of chlorophenolic compounds with pyrite-Fenton process
    (Elsevier Sci Ltd, 2019) Kantar, Cetin; Oral, Ozlem; Urken, Ozge; Oz, Nilgun Ayman; Keskin, Selda
    Batch experiments, in conjunction with chromatographic and spectroscopic measurements, were performed to comparatively investigate the degradation of various chlorophenolic (CP) compounds (e.g., 2-CP, 4-CP, 2,3-DCP, 2,4-DCP, 2,4,6-TCP, 2,3,4,6-TeCP) by a modified Fenton process using pyrite as the catalyst The batch results show that the CP removal by pyrite-Fenton process was highly dependent on chemical conditions (e.g., pH, CP and pyrite concentration), CP type, number and location of chlorine atoms on the aromatic ring. With the exception of 2,3,4,6-TeCP and 2,3-DCP, the CP removal decreased with increasing the number of chlorine constituents. While the main mechanism responsible for monochlorophenol removal (e.g., 2-CP and 4-CP) was the hydroxyl radical attack on aromatic rings, the CP removal for multichlorophenolic compounds (e.g., 2,3,4,6-TeCP) was driven by both: (1) hydroxyl radical attack on aromatic rings by both solution and surface-bound hydroxyl radicals and (2) adsorption onto pyrite surface sites. The adsorption affinity increased with increasing the number of Cl atoms on the aromatic ring due to enhanced hydrophobic effect. The TOC removal was not 100% complete for all CPs investigated due to formation of chemically less degradable chlorinated intermediate organic compounds as well as low molecular weight organic acids such as formic and acetic acid. Spectroscopic measurements with SEM-EDS, zeta potential and XPS provided evidence for the partial oxidation of pyrite surface Fe(II) and disulfide groups under acidic conditions. (C) 2019 Elsevier Ltd. All rights reserved.
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    Role of complexing agents on oxidative degradation of chlorophenolic compounds by pyrite-Fenton process: Batch and column experiments
    (Elsevier Science Bv, 2019) Kantar, Cetin; Oral, Ozlem; Urken, Ozge; Oz, Nilgun Ayman
    This study involves batch reactor and fixed-bed continuous flow experiments to determine the effects of complexing agents (e.g., tartrate and citrate) on the treatment of chlorophenolic (CP) compounds using heterogeneous Fenton system with pyrite mineral as the iron source. While the addition of organic ligands to the batch systems adversely affected CP removal, organic ligands had a beneficial effect on CP removal in column systems. Although the ligands extended the life span of pyrite-packed columns by removing surface oxidation products through the formation of soluble Fe-ligand complexes, the ligands competed against CPs for hydroxyl radicals (HO*). The competitive effect was much higher in batch systems since pyrite loading was very low in order to generate sufficient hydroxyl radicals. On the other hand, at much higher pyrite loading of column experiments, the H* radicals generated during Fenton process were sufficient to overcome the competitive effect exerted by organic ligands. In spite of much higher Fe solubility in the presence of citrate, citrate was less effective in enhancing CP removal in column systems compared to tartrate since the competitive effect caused by citrate for HO* radicals was more than that exerted by tartrate.
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    Role of reactor type on Cr(VI) removal by zero-valent iron in the presence of pyrite: Batch versus sequential batch reactors
    (Academic Press Ltd- Elsevier Science Ltd, 2022) Oral, Ozlem; Yigit, Aynur; Kantar, Cetin
    This study was conducted to understand the role of application sequence of pyrite and zero-valent iron (Fe0) (simultaneous vs. sequential) on chromium (VI) removal by Fe0. In batch experiments, pyrite and Fe0 were homogeneously mixed in batch reactors maintained at a constant total solids loading of 2 g L-1. In sequential batch experiments, however, the first reactor containing variable doses of pyrite was operated for 20 min, and the liquid fraction from the first reactor was then subsequently loaded into the second reactor containing a fixed Fe0 dose of 1.2 g L-1. The batch reactors achieved much higher Cr(VI) removal efficiency than sequential batch reactors under similar operating conditions due to discrepancies in Fe redox cycling activities between these two systems. In batch reactors, the Fe0 particles deposited on pyrite surface due to electrostatic attraction between negatively charged pyrite and positively charged Fe0, thus, rendering the overall solids surface charge neutral at optimum pyrite and Fe0 doses. As a result, the whole system behaved like a composite material, with pyrite functioning as a support material for Fe0. This stimulated Fe redox cycling more effectively to generate new Fe(II) sites on Fe0 for enhanced Cr(VI) removal relative to Fe0 only system. In sequential batch reactors, however, the Fe redox cycling activity was limited, but significantly increased with increasing pyrite dose in the first reactor. Overall, our results indicate that the stimulatory effect of pyrite on Cr(VI) removal by Fe0 may be much higher if the reactors are operated in batch mode.