Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs
Abstract Recently, the wide application of CuO nanoparticles (NPs) in engineering field inevitably leads to its release into various geologic settings, which has aroused great concern about the geochemical behaviors of CuO NPs due to its high surface reactivity and impact on the fate of co-existing...
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doaj-835ef574f9c04329881866cd5477f4a62020-11-25T01:07:40ZengBMCGeochemical Transactions1467-48662018-06-0119111210.1186/s12932-018-0058-3Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHsLingqun Zeng0Biao Wan1Rixiang Huang2Yupeng Yan3Xiaoming Wang4Wenfeng Tan5Fan Liu6Xionghan Feng7Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversitySchool of Earth and Atmospheric Sciences, Georgia Institute of TechnologyKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityKey Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture College of Resources and Environment, Huazhong Agricultural UniversityAbstract Recently, the wide application of CuO nanoparticles (NPs) in engineering field inevitably leads to its release into various geologic settings, which has aroused great concern about the geochemical behaviors of CuO NPs due to its high surface reactivity and impact on the fate of co-existing contaminants. However, the redox transformation of pollutants mediated by CuO NPs and the underlying mechanism still remain poorly understood. Here, we studied the interaction of CuO NPs with As(III), and explored the reaction pathways using batch experiments and multiple spectroscopic techniques. The results of in situ quick scanning X-ray absorption spectroscopy (Q-XAS) analysis verified that CuO NPs is capable of catalytically oxidize As(III) under dark conditions efficiently at a wide range of pHs. As(III) was firstly adsorbed on CuO NPs surface and then gradually oxidized to As(V) with dissolved O2 as the terminal electron acceptor. As(III) adsorption increased to the maximum at a pH close to PZC of CuO NPs (~ pH 9.2), and then sharply decreased with increasing pH, while the oxidation capacity monotonically increased with pH. X-ray photoelectron spectroscopy and electron paramagnetic resonance characterization of samples from batch experiments indicated that two pathways may be involved in As(III) catalytic oxidation: (1) direct electron transfer from As(III) to Cu(II), followed by concomitant re-oxidation of the produced Cu(I) by dissolved O2 back to Cu(II) on CuO NPs surface, and (2) As(III) oxidation by reactive oxygen species (ROS) produced from the above Cu(I) oxygenation process. These observations facilitate a better understanding of the surface catalytic property of CuO NPs and its interaction with As(III) and other elements with variable valence in geochemical environments.http://link.springer.com/article/10.1186/s12932-018-0058-3CuO NPsAs(III)OxidationAdsorptionSurface catalysis |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Lingqun Zeng Biao Wan Rixiang Huang Yupeng Yan Xiaoming Wang Wenfeng Tan Fan Liu Xionghan Feng |
spellingShingle |
Lingqun Zeng Biao Wan Rixiang Huang Yupeng Yan Xiaoming Wang Wenfeng Tan Fan Liu Xionghan Feng Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs Geochemical Transactions CuO NPs As(III) Oxidation Adsorption Surface catalysis |
author_facet |
Lingqun Zeng Biao Wan Rixiang Huang Yupeng Yan Xiaoming Wang Wenfeng Tan Fan Liu Xionghan Feng |
author_sort |
Lingqun Zeng |
title |
Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs |
title_short |
Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs |
title_full |
Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs |
title_fullStr |
Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs |
title_full_unstemmed |
Catalytic oxidation of arsenite and reaction pathways on the surface of CuO nanoparticles at a wide range of pHs |
title_sort |
catalytic oxidation of arsenite and reaction pathways on the surface of cuo nanoparticles at a wide range of phs |
publisher |
BMC |
series |
Geochemical Transactions |
issn |
1467-4866 |
publishDate |
2018-06-01 |
description |
Abstract Recently, the wide application of CuO nanoparticles (NPs) in engineering field inevitably leads to its release into various geologic settings, which has aroused great concern about the geochemical behaviors of CuO NPs due to its high surface reactivity and impact on the fate of co-existing contaminants. However, the redox transformation of pollutants mediated by CuO NPs and the underlying mechanism still remain poorly understood. Here, we studied the interaction of CuO NPs with As(III), and explored the reaction pathways using batch experiments and multiple spectroscopic techniques. The results of in situ quick scanning X-ray absorption spectroscopy (Q-XAS) analysis verified that CuO NPs is capable of catalytically oxidize As(III) under dark conditions efficiently at a wide range of pHs. As(III) was firstly adsorbed on CuO NPs surface and then gradually oxidized to As(V) with dissolved O2 as the terminal electron acceptor. As(III) adsorption increased to the maximum at a pH close to PZC of CuO NPs (~ pH 9.2), and then sharply decreased with increasing pH, while the oxidation capacity monotonically increased with pH. X-ray photoelectron spectroscopy and electron paramagnetic resonance characterization of samples from batch experiments indicated that two pathways may be involved in As(III) catalytic oxidation: (1) direct electron transfer from As(III) to Cu(II), followed by concomitant re-oxidation of the produced Cu(I) by dissolved O2 back to Cu(II) on CuO NPs surface, and (2) As(III) oxidation by reactive oxygen species (ROS) produced from the above Cu(I) oxygenation process. These observations facilitate a better understanding of the surface catalytic property of CuO NPs and its interaction with As(III) and other elements with variable valence in geochemical environments. |
topic |
CuO NPs As(III) Oxidation Adsorption Surface catalysis |
url |
http://link.springer.com/article/10.1186/s12932-018-0058-3 |
work_keys_str_mv |
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