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Degradation of aqueous 2,4,4'-Trihydroxybenzophenone by persulfate activated with nitrogen doped carbonaceous materials and the formation of dimer products.

Authors
  • Pan, Xiaoxue1
  • Chen, Jing1
  • Wu, Nannan1
  • Qi, Yumeng1
  • Xu, Xinxin1
  • Ge, Jiali1
  • Wang, Xinghao1
  • Li, Chenguang1
  • Qu, Ruijuan2
  • Sharma, Virender K3
  • Wang, Zunyao1
  • 1 State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, Jiangsu 210023, PR China. , (China)
  • 2 State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, Jiangsu 210023, PR China. Electronic address: [email protected] , (China)
  • 3 Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, College Station, TX 77843, USA.
Type
Published Article
Journal
Water research
Publication Date
Oct 15, 2018
Volume
143
Pages
176–187
Identifiers
DOI: 10.1016/j.watres.2018.06.038
PMID: 29945033
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

In this work, we systematically investigated the persulfate (PS) activation potential of a series of nitrogen doped carbonaceous materials for the degradation of 2,4,4'-trihydroxybenzophenone (2,4,4'-HBP), an additive in polyvinyl acetate films and personal care products. Nitrogen originating from urea, NH4NO3, indole and polyaniline was doped into carbonaceous materials, including hydroxylated multi-walled carbon nanotubes (CNT-OH), large-inner thin-walled carboxylated carbon nanotubes (CNT-COOH) and graphite oxide (GO), to examine the catalytic effect. The NH4NO3-CNT-OH catalyst, which showed the best catalytic performance in 2,4,4'-HBP removal, was characterized by SEM, TEM, FT-IR, Raman, BET surface area, XRD and XPS, and pyrrolic nitrogen was found to play a highly important role in the activation of PS. Under the conditions of [2,4,4'-HBP]0: [PS]0 = 1: 500, T = 25 °C, pH0 = 7.0, concentration of catalyst = 100 mg L-1, 43.48 μM 2,4,4'-HBP was completely removed in 2 h. According to electron paramagnetic resonance (EPR) spectra and radical quenching experiments, hydroxyl and sulfate radicals on the surface of the catalyst contributed to the substrate oxidation. Cleavage of C-C bridge bond, hydroxylation and polymerization were mainly involved in the oxidation process, leading to the formation of 10 intermediates (e.g., dimers), as detected by the MS/MS spectra. To the best of our knowledge, this report is the first to describe the transformation mechanism of 2,4,4'-HBP in nitrogen doped carbonaceous materials catalyzed PS system. Copyright © 2018 Elsevier Ltd. All rights reserved.

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