Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water

doi:10.1007/s11783-019-1170-z

Front. Environ. Sci. Eng.

2019, Vol. 13

Issue (6) : 86 https://doi.org/10.1007/s11783-019-1170-z

RESEARCH ARTICLE

Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water

Bei Ye¹, Zhuo Chen^2,³, Xinzheng Li², Jianan Liu^2,³, Qianyuan Wu²(

), Cheng Yang⁴(

), Hongying Hu^1,³, 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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Abstract

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 Author(s): 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.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1170-z
https://academic.hep.com.cn/fese/EN/Y2019/V13/I6/86

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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