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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2019, Vol. 13 Issue (6) : 86
Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water
Bei Ye1, Zhuo Chen2,3, Xinzheng Li2, Jianan Liu2,3, Qianyuan Wu2(), Cheng Yang4(), Hongying Hu1,3, Ronghe Wang2
1. Shenzhen Environmental Science and New Energy Technology Engineering Laboratory, Tsinghua-Berkeley Shenzhen Institute, Tsinghua University, Shenzhen 518055, China
2. Key Laboratory of Microorganism Application and Risk Control of Shenzhen, Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental Safety, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, China
3. Environmental Simulation and Pollution Control State Key Joint Laboratory, State Environmental Protection Key Laboratory of Microorganism Application and Risk Control (SMARC), School of Environment, Tsinghua University, Beijing 100084, China
4. Division of Energy and Environment, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, China
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GO or RGO promotes bromate formation during ozonation of bromide-containing water.

CeO2/RGO significantly inhibits bromate formation compared to RGO during ozonation.

CeO2/RGO shows an enhancement on DEET degradation efficiency during ozonation.

Ozone (O3) is widely used in drinking water disinfection and wastewater treatment. However, when applied to bromide-containing water, ozone induces the formation of bromate, which is carcinogenic. Our previous study found that graphene oxide (GO) can enhance the degradation efficiency of micropollutants during ozonation. However, in this study, GO was found to promote bromate formation during ozonation of bromide-containing waters, with bromate yields from the O3/GO process more than twice those obtained using ozone alone. The promoted bromate formation was attributed to increased hydroxyl radical production, as confirmed by the significant reduction (almost 75%) in bromate yield after adding t-butanol (TBA). Cerium oxide (less than 5 mg/L) supported on reduced GO (xCeO2/RGO) significantly inhibited bromate formation during ozonation compared with reduced GO alone, and the optimal Ce atomic percentage (x) was determined to be 0.36%, achieving an inhibition rate of approximately 73%. Fourier transform infrared (FT-IR) spectra indicated the transformation of GO into RGO after hydrothermal treatment, and transmission electron microscope (TEM) results showed that CeO2 nanoparticles were well dispersed on the RGO surface. The X-ray photoelectron spectroscopy (XPS) spectra results demonstrated that the Ce3+/Ce4+ ratio in xCeO2/RGO was almost 3‒4 times higher than that in pure CeO2, which might be attributed to the charge transfer effect from GO to CeO2. Furthermore, Ce3+ on the xCeO2/RGO surface could quench Br and BrO to further inhibit bromate formation. Meanwhile, 0.36CeO2/RGO could also enhance the degradation efficiency of N,N-diethyl-m-toluamide (DEET) in synthetic and reclaimed water during ozonation.

Keywords Bromate      Catalytic ozonation      Graphene oxide      Cerium dioxide     
Corresponding Authors: Qianyuan Wu,Cheng Yang   
Issue Date: 19 November 2019
 Cite this article:   
Bei Ye,Zhuo Chen,Xinzheng Li, et al. Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water[J]. Front. Environ. Sci. Eng., 2019, 13(6): 86.
Fig.1  (a)?(c) TEM  images of 0.36CeO2/RGO, (d) The size distribution of CeO2 dispersed on the surface of RGO.
Fig.2  The atomic  percentage of Ce element in catalysts by XPS.
Fig.3  (a) Change of Br - and BrO3- concentrations in synthetic water during O3 and O3/GO processes, (b) The effect of tBuOH on bromate formation during O3/GO process. Experimental conditions: [Br-] = 12.5?M, [O3] = 10 mg/(L·min), [GO] = 20 mg/L, [tBuOH] = 320?M, and pH= 7 with 10 mM PBS. Reaction time was 10 min.
Fig.4  The effect of  xCeO2/RGO hybrids on bromate formation in synthetic water during catalytic ozonation. (a) Dependence of bromate concentration on xCeO2/RGO, (b) Dependence of BrO3? and Br? concentrations on xCeO2/RGO. Experimental conditions: [Br?] = 12.5 ?M, [O3] = 10 mg/(L·min), [RGO] = 20 mg/L, [xCeO2/RGO] = 20 mg/L, [CeO2] = 500 mg/L, pH= 7 with 10 mM PBS. Reaction time was 10 min.
Fig.5  Bromate formation  in reclaimed water during ozonation. (a) Change of bromide concentration, (b) Change of bromate concentration. Experimental conditions: [Br?] = 12.5?M, [O3] = 10 mg/(L·min), [0.36CeO2/GO] = 20 mg/L, GO= 20 mg/L.
Fig.6  Degradation efficiency  of DEET by ozonation and catalytic ozonation. Experimental conditions: (a) in synthetic water: [DEET] = 50 ?M, [O3] = 10 mg/(L·min), [0.36CeO2/GO] = 20 mg/L, GO= 20 mg/L, [PBS] = 10 mM, pH= 7; (b) in reclaimed water: [DEET] = 0.52?M, [O3] = 10 mg/(L·min), [0.36CeO2/GO] = 20 mg/L, GO= 20 mg/L.
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