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Peroxymonosulfate activation by iron(III)-tetraamidomacrocyclic ligand for degradation of organic pollutants via high-valent iron-oxo complex
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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Buxton, G. V., Greenstock, C. L., Helman, W. P., & Ross, A. B. (1988) · Journal of Physical and Chemical Reference Data · doi:10.1063/1.555805 · Cited by 12,332
Yun, E.-T., Lee, J. H., Kim, J., Park, H.-D., & Lee, J. (2018) · Environmental Science & Technology · doi:10.1021/acs.est.8b00959 · Cited by 1,175
Cited by
Peng, L., Duan, X., Shang, Y., Gao, B., & Xu, X. (2021) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2021.119963 · Cited by 485
Li, Y., Yang, T., Qiu, S., Lin, W., Yan, J., Fan, S., & Zhou, Q. (2020) · Chemical Engineering Journal · doi:10.1016/j.cej.2020.124382 · Cited by 365
Huang, B., Wu, Z., Wang, X., Song, X., Zhou, H., Zhang, H., Zhou, P., Liu, W., Xiong, Z., & Lai, B. (2023) · Environmental Science & Technology · doi:10.1021/acs.est.3c05509 · Cited by 281
Zhou, X., Zhao, Q., Wang, J., Chen, Z., & Chen, Z. (2021) · Chemical Engineering Journal · doi:10.1016/j.cej.2020.128312 · Cited by 269
Metadata
- Authors
- Li, H., Shan, C., Li, W., & Pan, B.
- Venue
- Water Research
- Publisher
- Elsevier BV
- Published
- 2018-12
- Volume
- 147
- Pages
- 233-241
- ISSN
- 0043-1354 (ISSN-L)
- OpenAlex
- W2894981861
- Cited by
- 221
- References
- 2
- FWCI
- 8.91
- Type
- journal article
- Language
- en
- Open access
- closed
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- 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. https://doi.org/10.1016/j.watres.2018.10.015
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