Enhanced Oxidation of Organic Contaminants by Iron(II)-Activated Periodate: The Significance of High-Valent Iron–Oxo Species
العنوان: | Enhanced Oxidation of Organic Contaminants by Iron(II)-Activated Periodate: The Significance of High-Valent Iron–Oxo Species |
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المؤلفون: | Zhenyu Zhao, Binbin Shao, Yang Zong, Deli Wu, Yufei Shao, Longqian Xu, Wen Liu, Yunqiao Zeng |
المصدر: | Environmental Science & Technology. 55:7634-7642 |
بيانات النشر: | American Chemical Society (ACS), 2021. |
سنة النشر: | 2021 |
مصطلحات موضوعية: | High-valent iron, Ligand, Hydrogen bond, Iron, Periodic Acid, Inorganic chemistry, Periodate, Substrate (chemistry), Hydrogen Peroxide, General Chemistry, 010501 environmental sciences, 01 natural sciences, Potassium periodate, chemistry.chemical_compound, chemistry, Peroxydisulfate, Environmental Chemistry, Ferrous Compounds, Oxidation-Reduction, Iodate, 0105 earth and related environmental sciences |
الوصف: | Potassium periodate (PI, KIO4) was readily activated by Fe(II) under acidic conditions, resulting in the enhanced abatement of organic contaminants in 2 min, with the decay ratios of the selected pollutants even outnumbered those in the Fe(II)/peroxymonosulfate and Fe(II)/peroxydisulfate processes under identical conditions. Both 18O isotope labeling techniques using methyl phenyl sulfoxide (PMSO) as the substrate and X-ray absorption near-edge structure spectroscopy provided conclusive evidences for the generation of high-valent iron-oxo species (Fe(IV)) in the Fe(II)/PI process. Density functional theory calculations determined that the reaction of Fe(II) with PI followed the formation of a hydrogen bonding complex between Fe(H2O)62+ and IO4(H2O)-, ligand exchange, and oxygen atom transfer, consequently generating Fe(IV) species. More interestingly, the unexpected detection of 18O-labeled hydroxylated PMSO not only favored the simultaneous generation of ·OH but also demonstrated that ·OH was indirectly produced through the self-decay of Fe(IV) to form H2O2 and the subsequent Fenton reaction. In addition, IO4- was not transformed into the undesired iodine species (i.e., HOI, I2, and I3-) but was converted to nontoxic iodate (IO3-). This study proposed an efficient and environmental friendly process for the rapid removal of emerging contaminants and enriched the understandings on the evolution mechanism of ·OH in Fe(IV)-mediated processes. |
تدمد: | 1520-5851 0013-936X |
DOI: | 10.1021/acs.est.1c00375 |
URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::139892ba66135082bf9f85530831d8ed https://doi.org/10.1021/acs.est.1c00375 |
Rights: | CLOSED |
رقم الانضمام: | edsair.doi.dedup.....139892ba66135082bf9f85530831d8ed |
قاعدة البيانات: | OpenAIRE |
تدمد: | 15205851 0013936X |
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DOI: | 10.1021/acs.est.1c00375 |