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

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Abstract

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.

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References

  • Buxton G V, Greenstock C L, Helman W P, Ross A B (1988). Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (· OH/· O− in aqueous solution. Journal of Physical and Chemical Reference Data, 17(2): 513–886

    Article  CAS  Google Scholar 

  • Cai W, Chen F, Shen X, Chen L, Zhang J (2010). Enhanced catalytic degradation of AO7 in the CeO2-H2O2 system with Fe3+ doping. Applied Catalysis B: Environmental, 101(1–2): 160–168

    Article  CAS  Google Scholar 

  • Campbell C T, Peden C H F (2005). Chemistry. Oxygen vacancies and catalysis on ceria surfaces. Science, 309(5735): 713–714

    Article  CAS  Google Scholar 

  • Dai Q, Bai S, Li H, Liu W, Wang X, Lu G (2015). Catalytic total oxidation of 1,2-dichloroethane over highly dispersed vanadia supported on CeO2 nanobelts. Applied Catalysis B: Environmental, 168–169: 141–155

    Article  Google Scholar 

  • Dongmei L, Zhiwei W, Qi Z, Fuyi C, Yujuan S, Xiaodong L (2015). Drinking water toxicity study of the environmental contaminant—Bromate. Regul Toxicol Pharmacol, 73(3): 802–810

    Article  Google Scholar 

  • Fischbacher A, Löppenberg K, von Sonntag C, Schmidt T C (2015). A new reaction pathway for bromite to bromate in the ozonation of bromide. Environmental Science & Technology, 49(19): 11714–11720

    Article  CAS  Google Scholar 

  • Gao W, Wu G, Janicke M T, Cullen D A, Mukundan R, Baldwin J K, Brosha E L, Galande C, Ajayan P M, More K L, Dattelbaum A M, Zelenay P (2014). Ozonated graphene oxide film as a protonexchange membrane. Angew Chem Int Ed Engl, 53(14): 3588–3593

    Article  CAS  Google Scholar 

  • Han Q, Wang H, Dong W, Liu T, Yin Y (2013). Formation and inhibition of bromate during ferrate (VI) — Ozone oxidation process. Separation and Purification Technology, 118: 653–658

    Article  CAS  Google Scholar 

  • Han T, Zhang Z (2015). Novel hydrolyzing synthesis of CeO2-RGO support for Pt electrocatalyst in direct methanol fuel cells. Materials Letters, 154: 177–179

    Article  CAS  Google Scholar 

  • Jiang L, Yao M, Liu B, Li Q, Liu R, Lv H, Lu S, Gong C, Zou B, Cui T, Liu B, Hu G, Wågberg T (2012). Controlled synthesis of CeO2/graphene nanocomposites with highly enhanced optical and catalytic properties. Journal of Physical Chemistry C, 116(21): 11741–11745

    Article  CAS  Google Scholar 

  • Jothinathan L, Hu J (2018). Kinetic evaluation of graphene oxide based heterogenous catalytic ozonation for the removal of ibuprofen. Water Research, 134: 63–73

    Article  CAS  Google Scholar 

  • Lai L, Peng J, Ren Y, Li J, Zhang Y, Lai B (2018). Catalytic ozonation of succinic acid in aqueous solution by Co/Al2O3-EPM: Performance, characteristics, and reaction mechanism. Environmental Engineering Science, 35(12): 1309–1321

    Article  CAS  Google Scholar 

  • Li W, Lu X, Xu K, Qu J, Qiang Z (2015). Cerium incorporated MCM-48 (Ce-MCM-48) as a catalyst to inhibit bromate formation during ozonation of bromide-containing water: Efficacy and mechanism. Water Research, 86: 2–8

    Article  CAS  Google Scholar 

  • Li X, Yi H, Zhang J, Feng J, Li F, Xue D, Zhang H, Peng Y, Mellors N J (2013). Fe3O4-graphene hybrids: Nanoscale characterization and their enhanced electromagnetic wave absorption in gigahertz range. Journal of Nanoparticle Research, 15(3): 1472

    Article  Google Scholar 

  • Liu J N, Chen Z, Wu Q Y, Li A, Hu H Y, Yang C (2016). Ozone/graphene oxide catalytic oxidation: a novel method to degrade emerging organic contaminant N,N-diethyl-m-toluamide (DEET). Scientific Reports, 6(1): 31405

    Article  CAS  Google Scholar 

  • Lu N, Wu X F, Zhou J Z, Huang X, Ding G J (2015). Bromate oxidized from bromide during sonolytic ozonation. Ultrasonics Sonochemistry, 22: 139–143

    Article  CAS  Google Scholar 

  • Nawrocki J, Kasprzyk-Hordern B (2010). The efficiency and mechanisms of catalytic ozonation. Applied Catalysis B: Environmental, 99(1–2): 27–42

    Article  CAS  Google Scholar 

  • Nie Y, Hu C, Li N, Yang L, Qu J (2014). Inhibition of bromate formation by surface reduction in catalytic ozonation of organic pollutants over β-FeOOH/Al2O3. Applied Catalysis B: Environmental, 147: 287–292

    Article  CAS  Google Scholar 

  • Nie Y, Li N, Hu C (2015). Enhanced inhibition of bromate formation in catalytic ozonation of organic pollutants over Fe-Al LDH/Al2O3. Separation and Purification Technology, 151: 256–261

    Article  CAS  Google Scholar 

  • Oulton R, Haase J P, Kaalberg S, Redmond C T, Nalbandian M J, Cwiertny D M (2015). Hydroxyl radical formation during ozonation of multiwalled carbon nanotubes: performance optimization and demonstration of a reactive CNT filter. Environmental Science & Technology, 49(6): 3687–3697

    Article  CAS  Google Scholar 

  • Pant B, Saud P S, Park M, Park S J, Kim H Y (2016). General one-pot strategy to prepare Ag-TiO2 decorated reduced graphene oxide nanocomposites for chemical and biological disinfectant. Journal of Alloys and Compounds, 671: 51–59

    Article  CAS  Google Scholar 

  • Pelle K, Wittmann M, Lovrics K, Noszticzius Z (2004). Mechanistic investigations on the Belousov-Zhabotinsky reaction with oxalic acid substrate. 2. Measuring and modeling the oxalic acid-bromine chain reaction and simulating the complete oscillatory system. Journal of Physical Chemistry A, 108(37): 7554–7562

    Article  CAS  Google Scholar 

  • Pinkernell U, Von Gunten U (2001). Bromate minimization during ozonation: mechanistic considerations. Environmental Science & Technology, 35(12): 2525–2531

    Article  CAS  Google Scholar 

  • Sánchez-Polo M, von Gunten U, Rivera-Utrilla J (2005). Efficiency of activated carbon to transform ozone into *OH radicals: Influence of operational parameters. Water Research, 39(14): 3189–3198

    Article  Google Scholar 

  • Shahidi D, Roy R, Azzouz A (2015). Advances in catalytic oxidation of organic pollutants—Prospects for thorough mineralization by natural clay catalysts. Applied Catalysis B: Environmental, 174–175: 277–292

    Article  Google Scholar 

  • Song Z, Wang M, Wang Z, Wang Y, Li R, Zhang Y, Liu C, Liu Y, Xu B, Qi F (2019a). Insights into heteroatom-doped graphene for catalytic ozonation: Active centers, reactive oxygen species evolution, and catalytic mechanism. Environmental Science & Technology, 53(9): 5337–5348

    Article  CAS  Google Scholar 

  • Song Z, Zhang Y, Liu C, Xu B, Qi F, Yuan D, Pu S (2019b). Insight into OH and O2formation in heterogeneous catalytic ozonation by delocalized electrons and surface oxygen-containing functional groups in layered-structure nanocarbons. Chemical Engineering Journal, 357: 655–666

    Article  CAS  Google Scholar 

  • Teixidó E, Piqué E, Gonzalez-Linares J, Llobet J M, Gómez-Catalán J (2015). Developmental effects and genotoxicity of 10 water disinfection by-products in zebrafish. Journal of Water and Health, 13(1): 54–66

    Article  Google Scholar 

  • Vecchietti J, Baltanás M A, Gervais C, Collins S E, Blanco G, Matz O, Calatayud M, Bonivardi A (2017). Insights on hydride formation over cerium-gallium mixed oxides: A mechanistic study for efficient H2 dissociation. Journal of Catalysis, 345: 258–269

    Article  CAS  Google Scholar 

  • von Gunten U (2003). Ozonation of drinking water: Part II. Disinfection and by-product formation in presence of bromide, iodide or chlorine. Water Research, 37(7): 1469–1487

    Article  CAS  Google Scholar 

  • Wang Q, Yang Z, Ma J, Wang J, Wang L, Guo M (2016). Study on the mechanism of cerium oxide catalytic ozonation for controlling the formation of bromate in drinking water. Desalination and Water Treatment, 57(33): 15533–15546

    Article  CAS  Google Scholar 

  • Wang W, Zhu Q, Qin F, Dai Q, Wang X (2018). Fe doped CeO2 nanosheets as Fenton-like heterogeneous catalysts for degradation of salicylic acid. Chemical Engineering Journal, 333: 226–239

    Article  CAS  Google Scholar 

  • Wu Q Y, Zhou Y T, Li W, Zhang X, Du Y, Hu H Y (2019). Underestimated risk from ozonation of wastewater containing bromide: Both organic byproducts and bromate contributed to the toxicity increase. Water Research, 162: 43–52

    Article  CAS  Google Scholar 

  • Wu Y, Wu C, Wang Y, Hu C (2014). Inhibition of nano-metal oxides on bromate formation during ozonation process. Ozone Science and Engineering, 36(6): 549–559

    Article  Google Scholar 

  • Xingyi W, Qian K, Dao L (2009). Catalytic combustion of chlorobenzene over MnOx-CeO2 mixed oxide catalysts. Applied Catalysis B: Environmental, 86(3–4): 166–175

    Article  Google Scholar 

  • Xu Z, Xie M, Ben Y, Shen J, Qi F, Chen Z (2019). Efficiency and mechanism of atenolol decomposition in Co-FeOOH catalytic ozonation. Journal of Hazardous Materials, 365: 146–154

    Article  CAS  Google Scholar 

  • Yang J, Zhang H, Zhang Z, Lai B (2019). Degradation of 2,4-dinitrophenol in aqueous solution by microscale Fe0/H2O2/O3 process. Environmental Engineering Science, 36(2): 207–218

    Article  CAS  Google Scholar 

  • Ye Z, Tai H, Xie T, Yuan Z, Liu C, Jiang Y (2016). Room temperature formaldehyde sensor with enhanced performance based on reduced graphene oxide/titanium dioxide. Sensors and Actuators. B, Chemical, 223: 149–156

    Article  CAS  Google Scholar 

  • Zhang T, Chen W, Ma J, Qiang Z (2008). Minimizing bromate formation with cerium dioxide during ozonation of bromide-containing water. Water Research, 42(14): 3651–3658

    Article  CAS  Google Scholar 

  • Zhang L H, Zhou J, Liu Z Q, Guo J B (2019). Mesoporous CeO2 catalyst synthesized by using cellulose as template for the Ozonation of phenol. Ozone: Science and Engineering, 41(2): 166–174

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by grants from the National Key Research and Development Program of China (No.2016YFE0118800), the National Science Fund of China (Nos. 51578310), the Special Support Program for High-Level Personnel Recruitment in Guangdong Province (No.2016TQ03Z384), the Shenzhen Science, Technology and Innovation Commission (No. JCYJ20170818091859147), and the Water Cycle Program of Development and Reform Commission of Shenzhen Municipality.

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Authors and Affiliations

  1. Shenzhen Environmental Science and New Energy Technology Engineering Laboratory, Tsinghua-Berkeley Shenzhen Institute, Tsinghua University, Shenzhen, 518055, China

    Bei Ye & Hongying Hu

  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

    Zhuo Chen, Xinzheng Li, Jianan Liu, Qianyuan Wu & Ronghe Wang

  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

    Zhuo Chen, Jianan Liu & Hongying Hu

  4. Division of Energy and Environment, Graduate School at Shenzhen, Tsinghua University, Shenzhen, 518055, China

    Cheng Yang

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  1. Bei Ye
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  2. Zhuo Chen
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  3. Xinzheng Li
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  4. Jianan Liu
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  5. Qianyuan Wu
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  6. Cheng Yang
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  7. Hongying Hu
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  8. Ronghe Wang
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Correspondence to Qianyuan Wu or Cheng Yang.

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Highlights

• 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.

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Ye, B., Chen, Z., Li, X. et al. Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water. Front. Environ. Sci. Eng. 13, 86 (2019). https://doi.org/10.1007/s11783-019-1170-z

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  • DOI: https://doi.org/10.1007/s11783-019-1170-z

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