4.7 Article

Enhancing Fenton-like process at neutral pH by Fe(III)-GLDA complexation for the oxidation removal of organic pollutants

期刊

JOURNAL OF HAZARDOUS MATERIALS
卷 416, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.jhazmat.2021.126077

关键词

Fe(III) mediated Fenton-like reaction; Neutral pH; GLDA; Pollutants oxidation removal

资金

  1. National Key Research and Development Program of China [2020YFC1808301]
  2. Research on Water Environmental Protection Strategy and Management Policy in Beijing-Tianjin-Hebei Region [2018ZX07111001]
  3. Scientific Frontier and Interdisciplinary Research Project of Jilin University, Outstanding Youth Cultivation Plan of Jilin University
  4. Key Laboratory of Groundwater Resources and Environmental of Ministry of Education (Jilin University)
  5. State-Local joint engineering lab for control and remediation technologies of petrochemical contaminated site

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Utilizing N,N-bis(carboxymethyl)glutamic acid (GLDA) in Fe(III) mediated Fenton-like oxidation significantly enhances the removal of organic pollutants at neutral pH. The acceleration of the Fe(III)/Fe(II) cycle caused by GLDA contributes to the increased degradation rate of pollutants, especially ciprofloxacin (CIP), in the GLDA/Fe(III)/H2O2 system. The complexation of GLDA with Fe(III) modifies the redox potential and enhances the generation of hydroxyl radicals, leading to efficient pollutant degradation.
N,N-bis(carboxymethyl)glutamic acid (GLDA) was utilized in this study to significantly enhance the Fe(III) mediated Fenton-like oxidation removal of organic pollutants at neutral pH, in which ciprofloxacin (CIP) was used as the model pollutant. The CIP degradation rate in the GLDA/Fe(III)/H2O2 system reached 96.5% within 180 min and was nearly 14 times higher than that in the Fe(III)/H2O2 system. This enhancement was contributed to the acceleration of the cycle of Fe(III)/Fe(II) caused by GLDA, which was verified by UV-vis spectroscopy, cyclic voltammetry, and radical quenching experiments. The results proved that the GLDA could complex with Fe (III) and greatly modify the redox potential of Fe(III)/Fe(II). Moreover, radical quenching experiments confirmed that center dot OH and O-2(center dot-) were the mainly species for CIP degradation, and O-2(center dot-) was responsible for 81.9% center dot OH generation. In addition, H2O2 utilization kinetic modeling was also investigated. The optimum parameters of the 100 mu M Fe(III)-GLDA complex and 15 mM H2O2 were attained by lot-size optimization experiments. Two possible CIP degradation pathways were proposed on the basis of the intermediates identified by MS/MS. The GLDA/Fe(III)/H2O2 system performed better than common chelating agents at the same condition, manifesting good potential for environmental concerns.

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