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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.

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Publisher Full Text (DOI)

Authors+Show Affiliations

Li H
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China.
Shan C
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.
Li W
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.
Pan B
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.

MeSH

Environmental PollutantsHydrogen PeroxideIronPeroxides

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_ DB - PRIME DP - Unbound Medicine ER -