DOI: 10.1016/j.watres.2018.10.015
Scopus记录号: 2-s2.0-85054587665
论文题名: Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex
作者: Li H. ; Shan C. ; Li W. ; Pan B.
刊名: Water Research
ISSN: 431354
出版年: 2018
卷: 147 起始页码: 233
结束页码: 241
语种: 英语
英文关键词: Catalytic oxidation
; High-valent iron-oxo complex
; Iron(III)-tetraamidomacrocyclic ligand
; Nonradical pathway
; Peroxymonosulfate
英文摘要: 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−, SO4 2−, 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. © 2018 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/112358
Appears in Collections: 气候减缓与适应
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作者单位: State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, 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
Recommended Citation:
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[J]. Water Research,2018-01-01,147