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Oxidation of micropollutants by visible light active graphitic carbon nitride and ferrate(VI): Delineating the role of surface delocalized electrons.
Chemosphere. 2022 Nov; 307(Pt 2):135886.C

Abstract

The treatment of recalcitrant micropollutants in water remains challenging. Ferrate(VI) (FeVIO42-, Fe(VI)) has emerged as a green oxidant to oxidize organic molecules, however, its reactivity with recalcitrant micropollutants are sluggish. Our results demonstrate enhanced oxidation of carbamazepine (CBZ) by three types of visible light-responsive graphitic carbon nitride (g-C3N4) photocatalyst in absence and presence of ferrate(VI) (FeVIO42-, Fe(VI)) under mild alkaline conditions. The g-C3N4 photocatalysts were prepared by thermal process using urea, thiourea, and melamine and were named as CN-U, CN-T, and CN-M, respectively. The degradation efficiency of CBZ, in both visible light-g-C3N4 and visible light-g-C3N4-FeVIO42- systems followed the order of CN-U > CN-T > CN-M. The mechanisms for this trend was elucidated by measuring physiochemical properties of the microstructures with various surface and analytical techniques. Results suggest the dominating role of specific surface area and surface delocalized electrons of microstructures in degrading CBZ. Crystallinity, morphology, and surface functional groups may not directly associate with CBZ degradation. The CN-U has higher specific surface area and surface delocalized electrons than CN-T and CN-M and therefore the highest degradation efficiency of CBZ. The surface electrons likely generated O2●- and 1O2 in the visible light-g-C3N4 system. The additional oxidants, FeV and FeIV in the visible light-g-C3N4- FeVIO42- system led to higher degradation efficiency than the visible light-g-C3N4 system. Results suggest that the surfaces of g-C3N4 may be prepared preferentially with high levels of delocalized electrons at the surface of microstructures to enhance degradation of micropollutants.

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Publisher Full Text (DOI)

Authors+Show Affiliations

Pan B
Key Laboratory of Chemical Additives for China National Light Industry, School of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, PR China; Program for the Environment and Sustainability, Department of Environment and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Rd., College Station, TX, 77843, USA.
Zhou L
Key Laboratory of Chemical Additives for China National Light Industry, School of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, PR China.
Qin J
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, PR China.
Wang C
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, PR China.
Ma X
Department of Civil and Environmental Engineering, Texas A&M University, College Station, TX, 77843, USA.
Sharma VK
Program for the Environment and Sustainability, Department of Environment and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Rd., College Station, TX, 77843, USA. Electronic address: vshrma@tamu.edu.

MeSH

CarbamazepineCatalysisElectronsGraphiteIronLightNitrogen CompoundsOxidantsThioureaUreaWater

Pub Type(s)

Journal Article

Language

eng

PubMed ID

35926741

Citation

Pan, Bao, et al. "Oxidation of Micropollutants By Visible Light Active Graphitic Carbon Nitride and ferrate(VI): Delineating the Role of Surface Delocalized Electrons." Chemosphere, vol. 307, no. Pt 2, 2022, p. 135886.
Pan B, Zhou L, Qin J, et al. Oxidation of micropollutants by visible light active graphitic carbon nitride and ferrate(VI): Delineating the role of surface delocalized electrons. Chemosphere. 2022;307(Pt 2):135886.
Pan, B., Zhou, L., Qin, J., Wang, C., Ma, X., & Sharma, V. K. (2022). Oxidation of micropollutants by visible light active graphitic carbon nitride and ferrate(VI): Delineating the role of surface delocalized electrons. Chemosphere, 307(Pt 2), 135886. https://doi.org/10.1016/j.chemosphere.2022.135886
Pan B, et al. Oxidation of Micropollutants By Visible Light Active Graphitic Carbon Nitride and ferrate(VI): Delineating the Role of Surface Delocalized Electrons. Chemosphere. 2022;307(Pt 2):135886. PubMed PMID: 35926741.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Oxidation of micropollutants by visible light active graphitic carbon nitride and ferrate(VI): Delineating the role of surface delocalized electrons. AU - Pan,Bao, AU - Zhou,Linxing, AU - Qin,Jiani, AU - Wang,Chuanyi, AU - Ma,Xingmao, AU - Sharma,Virender K, Y1 - 2022/08/01/ PY - 2022/05/28/received PY - 2022/07/12/revised PY - 2022/07/27/accepted PY - 2022/8/5/pubmed PY - 2022/9/28/medline PY - 2022/8/4/entrez KW - Carbon nitride KW - Enhanced treatment KW - High-valent iron KW - Surface delocalized electrons KW - Visible light photocatalysis SP - 135886 EP - 135886 JF - Chemosphere JO - Chemosphere VL - 307 IS - Pt 2 N2 - The treatment of recalcitrant micropollutants in water remains challenging. Ferrate(VI) (FeVIO42-, Fe(VI)) has emerged as a green oxidant to oxidize organic molecules, however, its reactivity with recalcitrant micropollutants are sluggish. Our results demonstrate enhanced oxidation of carbamazepine (CBZ) by three types of visible light-responsive graphitic carbon nitride (g-C3N4) photocatalyst in absence and presence of ferrate(VI) (FeVIO42-, Fe(VI)) under mild alkaline conditions. The g-C3N4 photocatalysts were prepared by thermal process using urea, thiourea, and melamine and were named as CN-U, CN-T, and CN-M, respectively. The degradation efficiency of CBZ, in both visible light-g-C3N4 and visible light-g-C3N4-FeVIO42- systems followed the order of CN-U > CN-T > CN-M. The mechanisms for this trend was elucidated by measuring physiochemical properties of the microstructures with various surface and analytical techniques. Results suggest the dominating role of specific surface area and surface delocalized electrons of microstructures in degrading CBZ. Crystallinity, morphology, and surface functional groups may not directly associate with CBZ degradation. The CN-U has higher specific surface area and surface delocalized electrons than CN-T and CN-M and therefore the highest degradation efficiency of CBZ. The surface electrons likely generated O2●- and 1O2 in the visible light-g-C3N4 system. The additional oxidants, FeV and FeIV in the visible light-g-C3N4- FeVIO42- system led to higher degradation efficiency than the visible light-g-C3N4 system. Results suggest that the surfaces of g-C3N4 may be prepared preferentially with high levels of delocalized electrons at the surface of microstructures to enhance degradation of micropollutants. SN - 1879-1298 UR - https://www.unboundmedicine.com/medline/citation/35926741/Oxidation_of_micropollutants_by_visible_light_active_graphitic_carbon_nitride_and_ferrate_VI_:_Delineating_the_role_of_surface_delocalized_electrons_ DB - PRIME DP - Unbound Medicine ER -