Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation

In this work, nano-bimetallic Co/Fe oxides with different stoichiometric Co/Fe ratios were prepared using a novel one-step solution combustion method. The nano-bimetallic Co/Fe oxides were used for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The stoichiometric efficien...

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Main Authors: Bao, Yueping, Oh, Wen-Da, Lim, Teik-Thye, Wang, Rong, Webster, Richard David, Hu, Xiao
Other Authors: School of Civil and Environmental Engineering
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/143837
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1438372021-02-15T05:27:44Z Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation Bao, Yueping Oh, Wen-Da Lim, Teik-Thye Wang, Rong Webster, Richard David Hu, Xiao School of Civil and Environmental Engineering School of Materials Science and Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Nanyang Environment and Water Research Institute Engineering::Civil engineering Nano-bimetallic Oxides Stoichiometric Efficiencies In this work, nano-bimetallic Co/Fe oxides with different stoichiometric Co/Fe ratios were prepared using a novel one-step solution combustion method. The nano-bimetallic Co/Fe oxides were used for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The stoichiometric efficiencies of the as-prepared nano-bimetallic catalysts were calculated and compared for the first time. The radical generation was identified by electron paramagnetic resonance (EPR) as well as chemical quenching experiments, in which different scavengers were used and compared. The catalytic PMS activation mechanism in the presence of catalyst was examined by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that besides SO4•- and •OH, •OOH was also detected in the PMS/CoFeO2.5 system. Meanwhile, in addition to the previously proposed radical oxidation pathway, the results showed that SMX degradation also involved a non-radical oxidation, which could be verified by the degradation experiment without catalyst as well as the detection of 1O2. In the PMS activation process, cobalt functioned as the active site on CoFeO2.5 while Fe oxide functioned as the adsorption site. The electron transfer mechanism was proposed based on the XPS and metal leaching results. Additionally, via the detection of transformation products, different SMX transformation pathways involving nitration, hydroxylation and hydrolysis in the PMS/CoFeO2.5 system were proposed. Accepted version 2020-09-25T04:44:24Z 2020-09-25T04:44:24Z 2019 Journal Article Bao, Y., Oh, W.-D., Lim, T.-T., Wang, R., Webster, R. D., & Hu, X. (2019). Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation. Water Research, 151, 64–74. doi:10.1016/j.watres.2018.12.007 0043-1354 https://hdl.handle.net/10356/143837 10.1016/j.watres.2018.12.007 30594091 151 64 74 en Water research © 2018 Elsevier Ltd. All rights reserved. This paper was published in Water research and is made available with permission of Elsevier Ltd. application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Civil engineering
Nano-bimetallic Oxides
Stoichiometric Efficiencies
spellingShingle Engineering::Civil engineering
Nano-bimetallic Oxides
Stoichiometric Efficiencies
Bao, Yueping
Oh, Wen-Da
Lim, Teik-Thye
Wang, Rong
Webster, Richard David
Hu, Xiao
Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
description In this work, nano-bimetallic Co/Fe oxides with different stoichiometric Co/Fe ratios were prepared using a novel one-step solution combustion method. The nano-bimetallic Co/Fe oxides were used for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The stoichiometric efficiencies of the as-prepared nano-bimetallic catalysts were calculated and compared for the first time. The radical generation was identified by electron paramagnetic resonance (EPR) as well as chemical quenching experiments, in which different scavengers were used and compared. The catalytic PMS activation mechanism in the presence of catalyst was examined by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that besides SO4•- and •OH, •OOH was also detected in the PMS/CoFeO2.5 system. Meanwhile, in addition to the previously proposed radical oxidation pathway, the results showed that SMX degradation also involved a non-radical oxidation, which could be verified by the degradation experiment without catalyst as well as the detection of 1O2. In the PMS activation process, cobalt functioned as the active site on CoFeO2.5 while Fe oxide functioned as the adsorption site. The electron transfer mechanism was proposed based on the XPS and metal leaching results. Additionally, via the detection of transformation products, different SMX transformation pathways involving nitration, hydroxylation and hydrolysis in the PMS/CoFeO2.5 system were proposed.
author2 School of Civil and Environmental Engineering
author_facet School of Civil and Environmental Engineering
Bao, Yueping
Oh, Wen-Da
Lim, Teik-Thye
Wang, Rong
Webster, Richard David
Hu, Xiao
format Article
author Bao, Yueping
Oh, Wen-Da
Lim, Teik-Thye
Wang, Rong
Webster, Richard David
Hu, Xiao
author_sort Bao, Yueping
title Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
title_short Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
title_full Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
title_fullStr Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
title_full_unstemmed Elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
title_sort elucidation of stoichiometric efficiency, radical generation and transformation pathway during catalytic oxidation of sulfamethoxazole via peroxymonosulfate activation
publishDate 2020
url https://hdl.handle.net/10356/143837
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