Ozonation of carbamazepine in the presence of sulfur-dopped graphene: Effect of process parameters and formation of main transformation products

被引:10
作者
Asghar, Anam [1 ]
Hammad, Mohaned [2 ]
Kerpen, Klaus [1 ]
Niemann, Felix [1 ]
Al-Kamal, Ahmed K. [3 ]
Segets, Doris [2 ,4 ]
Wiggers, Hartmut [3 ,4 ]
Schmidt, Torsten C. [1 ,5 ,6 ]
机构
[1] Univ Duisburg Essen, Fac Chem, Instrumental Analyt Chem, Univ Str 5, Essen, Germany
[2] Univ Duisburg Essen, Inst Combust & Gas Dynam Particle Sci & Technol IV, Duisburg, Germany
[3] Univ Duisburg Essen, Inst Combust & Gas Dynam React Fluids IVG RF, Duisburg, Germany
[4] Univ Duisburg Essen, Ctr Nanointegrat Duisburg Essen CENIDE, Duisburg, Germany
[5] Ctr Water & Environm Res ZWU, Univ Str 5, D-45141 Essen, Germany
[6] IWW Water Ctr, Moritzstr 26, D-45476 Mulheim An Der Ruhr, Germany
关键词
Catalytic ozonation; Hydroxyl radical; Microwave plasma; Sulfur-doped graphene; Transformation products; OXYGEN REDUCTION REACTION; CATALYTIC OZONATION; ADVANCED OXIDATION; DOPED GRAPHENE; WASTE-WATER; REMOVAL; OZONE; PEROXYMONOSULFATE; DEGRADATION; PERFORMANCE;
D O I
10.1016/j.scitotenv.2022.161079
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The stability of graphene structure in sulfur-doped graphene catalyst is demonstrated to be a key aspect during the ozonation process. Enhancing the stability of the sulfur-doped graphene structure is therefore important to improve its catalytic activity during the ozonation process. However, this has remained a challenge so far. Therefore, we adopted a low-energy microwave plasma technique to synthesize a high purity sulfur-doped graphene (S _ Gr) catalyst for the ozonation process. The effect of S _ Gr in the ozonation process was tested using carbamazepine (CBZ; 0.05 mM) as a probe compound. A complete CBZ removal was obtained at an ozone concentration of 0.08 mM while in comparison with single O3, similar to 1.5 and 2.5 times decrease in the formation of the two important in-termediate transformation products i.e., BQM (1-(2-benzaldehyde) - 4-hydroxy (1H, 3H)-quinazoline-2-one) and BQD (1-(2-benzaldehyde) -(1H, 3H)-quinazoline-2, 4-dione) was observed. Radical scavenging experiments confirmed the formation of HO center dot. The XPS results showed that the activity of S _ Gr towards the formation of HO center dot was positively related to S-bearing carbon atoms at the edge of the graphene structure. Therefore, the addition of S _ Gr is directly linked with the formation of HO center dot, which further contributed to the improved elimination of intermediate transforma-tion products. With a low sulfur loss of 1 %, the microwave plasma synthesized S _ Gr catalyst remained stable during ozonation, implying its feasibility in practical application.
引用
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页数:12
相关论文
共 57 条
[11]   Hydroxyl radical ozone ratios during ozonation processes.: I-The Rct concept [J].
Elovitz, MS ;
von Gunten, U .
OZONE-SCIENCE & ENGINEERING, 1999, 21 (03) :239-260
[12]   Adsorption and decomposition of water-dissolved ozone on high silica zeolites [J].
Fujita, H ;
Izumi, J ;
Sagehashi, M ;
Fujii, T ;
Sakoda, A .
WATER RESEARCH, 2004, 38 (01) :159-165
[13]   Catalytic ozonation of sulphamethoxazole in the presence of carbon materials: Catalytic performance and reaction pathways [J].
Goncalves, Alexandra G. ;
Orfao, Jose J. M. ;
Pereira, Manuel Fernando R. .
JOURNAL OF HAZARDOUS MATERIALS, 2012, 239 :167-174
[14]   Can the commonly used quenching method really evaluate the role of reactive oxygen species in pollutant abatement during catalytic ozonation? [J].
Guo, Yang ;
Long, Jingfei ;
Huang, Jun ;
Yu, Gang ;
Wang, Yujue .
WATER RESEARCH, 2022, 215
[15]   Comparison of emerging contaminant abatement by conventional ozonation, catalytic ozonation, O3/H2O2 and electro-peroxone processes [J].
Guo, Yang ;
Zhao, Erzhuo ;
Wang, Jun ;
Zhang, Xiaoyuan ;
Huang, Haiou ;
Yu, Gang ;
Wang, Yujue .
JOURNAL OF HAZARDOUS MATERIALS, 2020, 389
[16]   Role of oxygen functional groups in reduced graphene oxide for lubrication [J].
Gupta, Bhavana ;
Kumar, Niranjan ;
Panda, Kalpataru ;
Kanan, Vigneshwaran ;
Joshi, Shailesh ;
Visoly-Fisher, Iris .
SCIENTIFIC REPORTS, 2017, 7
[17]   Synthesis of novel LaCoO3/graphene catalysts as highly efficient peroxymonosulfate activator for the degradation of organic pollutants [J].
Hammad, Mohaned ;
Angel, Steven ;
Al-Kamal, Ahmed K. ;
Asghar, Anam ;
Amin, Amin Said ;
Kraeenbring, Mena-Alexander ;
Wiedemann, Haakon T. A. ;
Vinayakumar, Vineetha ;
Ali, Md Yusuf ;
Fortugno, Paolo ;
Kim, Cheolyong ;
Schmidt, Torsten C. ;
Kay, Christopher W. M. ;
Schulz, Christof ;
Segets, Doris ;
Wiggers, Hartmut .
CHEMICAL ENGINEERING JOURNAL, 2023, 454
[18]   A nanometer-ZnO catalyst to enhance the ozonation of 2,4,6-trichlorophenol in water [J].
Huang, WJ ;
Fang, GC ;
Wang, CC .
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 2005, 260 (1-3) :45-51
[19]   Ozonation products of carbamazepine and their removal from secondary effluents by soil aquifer treatment - Indications from column experiments [J].
Huebner, U. ;
Seiwert, B. ;
Reemtsma, T. ;
Jekel, M. .
WATER RESEARCH, 2014, 49 :34-43
[20]   Catalytic ozonation for the removal of organic contaminants in water on alumina [J].
Ikhlaq, Amir ;
Brown, David R. ;
Kasprzyk-Hordern, Barbara .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 165 :408-418