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Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex.
Water Res. 2018 12 15; 147:233-241.WR

Abstract

Herein, we proposed a new catalytic oxidation system, i.e., iron(III)-tetraamidomacrocyclic ligand (FeIII-TAML) mediated activation of peroxymonosulfate (PMS), for highly efficient organic degradation using p-chlorophenol (4-CP) as a model one. PMS/FeIII-TAML is capable of degrading 4-CP completely in 9 min at the initial 4-CP of 50 μM and pH = 7, whereas the recently explored system, H2O2/FeIII-TAML, could only result in ∼22% 4-CP removal in 20 min under otherwise identical conditions. More attractively, inorganic anions (i.e., Cl-, SO42-, NO3-, and HCO3-) exhibited insignificant effect on 4-CP degradation, and the negative effect of natural organic matters (NOM) on the degradation of 4-CP in PMS/FeIII-TAML is much weaker than the sulfate radical-based oxidation process (PMS/Co2+). Combined with in-situ XANES spectra, UV-visible spectra, electron paramagnetic resonance (EPR) spectra, and radical quenching experiments, high-valent iron-oxo complex (FeIV(O)TAML) instead of singlet oxygen (1O2), superoxide radical (O2•-), sulfate radicals (SO4•-) and hydroxyl radicals (HO•) was the key active species responsible for 4-CP degradation. The formation rate (kI) and consumption rate (kII) of the FeIV(O)TAML in PMS/FeIII-TAML were pH-dependent in the range of 6.0-11.5. As expected, increasing the FeIII-TAML and PMS dosage resulted in a higher steady-state concentration of FeIV(O)TAML and enhanced the 4-CP degradation accordingly. In addition, the oxidation capacity of PMS was almost totally utilized in PMS/FeIII-TAML for 4-CP oxidation due to the two-electron abstraction from 4-CP by one PMS. We believe this study will shed new light on effective PMS activation by Fe-ligand complexes to efficiently degrade organic contaminants via nonradical pathway.

Authors+Show Affiliations

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China.State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China; Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing, 210023, China.Key Laboratory of Surficial Geochemistry, Ministry of Education, School of Earth Sciences and Engineering, Nanjing University, Nanjing, 210023, China; Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing, 210023, China.State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China; Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing, 210023, China. Electronic address: bcpan@nju.edu.cn.

Pub Type(s)

Journal Article
Research Support, Non-U.S. Gov't

Language

eng

PubMed ID

30312796

Citation

Li, Hongchao, et al. "Peroxymonosulfate Activation By iron(III)-tetraamidomacrocyclic Ligand for Degradation of Organic Pollutants Via High-valent Iron-oxo Complex." Water Research, vol. 147, 2018, pp. 233-241.
Li H, Shan C, Li W, et al. Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex. Water Res. 2018;147:233-241.
Li, H., Shan, C., Li, W., & Pan, B. (2018). Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex. Water Research, 147, 233-241. https://doi.org/10.1016/j.watres.2018.10.015
Li H, et al. Peroxymonosulfate Activation By iron(III)-tetraamidomacrocyclic Ligand for Degradation of Organic Pollutants Via High-valent Iron-oxo Complex. Water Res. 2018 12 15;147:233-241. PubMed PMID: 30312796.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex. AU - Li,Hongchao, AU - Shan,Chao, AU - Li,Wei, AU - Pan,Bingcai, Y1 - 2018/10/06/ PY - 2018/07/10/received PY - 2018/09/30/revised PY - 2018/10/05/accepted PY - 2018/10/13/pubmed PY - 2019/9/26/medline PY - 2018/10/13/entrez KW - Catalytic oxidation KW - High-valent iron-oxo complex KW - Iron(III)-tetraamidomacrocyclic ligand KW - Nonradical pathway KW - Peroxymonosulfate SP - 233 EP - 241 JF - Water research JO - Water Res. VL - 147 N2 - Herein, we proposed a new catalytic oxidation system, i.e., iron(III)-tetraamidomacrocyclic ligand (FeIII-TAML) mediated activation of peroxymonosulfate (PMS), for highly efficient organic degradation using p-chlorophenol (4-CP) as a model one. PMS/FeIII-TAML is capable of degrading 4-CP completely in 9 min at the initial 4-CP of 50 μM and pH = 7, whereas the recently explored system, H2O2/FeIII-TAML, could only result in ∼22% 4-CP removal in 20 min under otherwise identical conditions. More attractively, inorganic anions (i.e., Cl-, SO42-, NO3-, and HCO3-) exhibited insignificant effect on 4-CP degradation, and the negative effect of natural organic matters (NOM) on the degradation of 4-CP in PMS/FeIII-TAML is much weaker than the sulfate radical-based oxidation process (PMS/Co2+). Combined with in-situ XANES spectra, UV-visible spectra, electron paramagnetic resonance (EPR) spectra, and radical quenching experiments, high-valent iron-oxo complex (FeIV(O)TAML) instead of singlet oxygen (1O2), superoxide radical (O2•-), sulfate radicals (SO4•-) and hydroxyl radicals (HO•) was the key active species responsible for 4-CP degradation. The formation rate (kI) and consumption rate (kII) of the FeIV(O)TAML in PMS/FeIII-TAML were pH-dependent in the range of 6.0-11.5. As expected, increasing the FeIII-TAML and PMS dosage resulted in a higher steady-state concentration of FeIV(O)TAML and enhanced the 4-CP degradation accordingly. In addition, the oxidation capacity of PMS was almost totally utilized in PMS/FeIII-TAML for 4-CP oxidation due to the two-electron abstraction from 4-CP by one PMS. We believe this study will shed new light on effective PMS activation by Fe-ligand complexes to efficiently degrade organic contaminants via nonradical pathway. SN - 1879-2448 UR - https://www.unboundmedicine.com/medline/citation/30312796/Peroxymonosulfate_activation_by_iron_III__tetraamidomacrocyclic_ligand_for_degradation_of_organic_pollutants_via_high_valent_iron_oxo_complex_ L2 - https://linkinghub.elsevier.com/retrieve/pii/S0043-1354(18)30809-1 DB - PRIME DP - Unbound Medicine ER -
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