Please wait a minute...
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    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 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
 Download: PDF(1456 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
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 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.
 URL:  
http://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1170-z
http://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.
1 G V Buxton, C L Greenstock, W P Helman, A B Ross (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
https://doi.org/10.1063/1.555805
2 W Cai, F Chen, X Shen, L Chen, J Zhang (2010). Enhanced catalytic degradation of AO7 in the CeO2–H2O2 system with Fe3+ doping. Applied Catalysis B: Environmental, 101(1–2): 160–168
https://doi.org/10.1016/j.apcatb.2010.09.031
3 C T Campbell, C H F Peden (2005). Chemistry. Oxygen vacancies and catalysis on ceria surfaces. Science, 309(5735): 713–714
https://doi.org/10.1126/science.1113955 pmid: 16051777
4 Q Dai, S Bai, H Li, W Liu, X Wang, G Lu (2015). Catalytic total oxidation of 1,2-dichloroethane over highly dispersed vanadia supported on CeO2 nanobelts. Applied Catalysis B: Environmental, 168–169: 141–155
https://doi.org/10.1016/j.apcatb.2014.12.028
5 L Dongmei, W Zhiwei, Z Qi, C Fuyi, S Yujuan, L Xiaodong (2015). Drinking water toxicity study of the environmental contaminant—Bromate. Regul Toxicol Pharmacol, 73(3): 802–810
https://doi.org/10.1016/j.yrtph.2015.10.015 pmid: 26496820
6 A Fischbacher, K Löppenberg, C von Sonntag, T C Schmidt (2015). A new reaction pathway for bromite to bromate in the ozonation of bromide. Environmental Science & Technology, 49(19): 11714–11720
https://doi.org/10.1021/acs.est.5b02634 pmid: 26371826
7 W Gao, G Wu, M T Janicke, D A Cullen, R Mukundan, J K Baldwin, E L Brosha, C Galande, P M Ajayan, K L More, A M Dattelbaum, P Zelenay (2014). Ozonated graphene oxide film as a proton-exchange membrane. Angew Chem Int Ed Engl, 53(14): 3588–3593
https://doi.org/10.1002/anie.201310908 pmid: 24677748
8 Q Han, H Wang, W Dong, T Liu, Y Yin (2013). Formation and inhibition of bromate during ferrate (VI) – Ozone oxidation process. Separation and Purification Technology, 118: 653–658
https://doi.org/10.1016/j.seppur.2013.07.042
9 T Han, Z Zhang (2015). Novel hydrolyzing synthesis of CeO2–RGO support for Pt electrocatalyst in direct methanol fuel cells. Materials Letters, 154: 177–179
https://doi.org/10.1016/j.matlet.2015.04.094
10 L Jiang, M Yao, B Liu, Q Li, R Liu, H Lv, S Lu, C Gong, B Zou, T Cui, B Liu, G Hu, T Wågberg (2012). Controlled synthesis of CeO2/graphene nanocomposites with highly enhanced optical and catalytic properties. Journal of Physical Chemistry C, 116(21): 11741–11745
https://doi.org/10.1021/jp3015113
11 L Jothinathan, J Hu (2018). Kinetic evaluation of graphene oxide based heterogenous catalytic ozonation for the removal of ibuprofen. Water Research, 134: 63–73
https://doi.org/10.1016/j.watres.2018.01.033 pmid: 29407652
12 L Lai, J Peng, Y Ren, J Li, Y Zhang, B Lai (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
https://doi.org/10.1089/ees.2018.0028
13 W Li, X Lu, K Xu, J Qu, Z Qiang (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
https://doi.org/10.1016/j.watres.2015.05.052 pmid: 26072989
14 X Li, H Yi, J Zhang, J Feng, F Li, D Xue, H Zhang, Y Peng, N J Mellors (2013). Fe3O4–graphene hybrids: Nanoscale characterization and their enhanced electromagnetic wave absorption in gigahertz range. Journal of Nanoparticle Research, 15(3): 1472
https://doi.org/10.1007/s11051-013-1472-1
15 J N Liu, Z Chen, Q Y Wu, A Li, H Y Hu, C Yang (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
https://doi.org/10.1038/srep31405 pmid: 27510858
16 N Lu, X F Wu, J Z Zhou, X Huang, G J Ding (2015). Bromate oxidized from bromide during sonolytic ozonation. Ultrasonics Sonochemistry, 22: 139–143
https://doi.org/10.1016/j.ultsonch.2014.05.024 pmid: 24931426
17 J Nawrocki, B Kasprzyk-Hordern (2010). The efficiency and mechanisms of catalytic ozonation. Applied Catalysis B: Environmental, 99(1–2): 27–42
https://doi.org/10.1016/j.apcatb.2010.06.033
18 Y Nie, C Hu, N Li, L Yang, J Qu (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
https://doi.org/10.1016/j.apcatb.2013.09.005
19 Y Nie, N Li, C Hu (2015). Enhanced inhibition of bromate formation in catalytic ozonation of organic pollutants over Fe–Al LDH/Al2O3. Separation and Purification Technology, 151: 256–261
https://doi.org/10.1016/j.seppur.2015.07.057
20 R Oulton, J P Haase, S Kaalberg, C T Redmond, M J Nalbandian, D M Cwiertny (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
https://doi.org/10.1021/es505430v pmid: 25730285
21 B Pant, P S Saud, M Park, S J Park, H Y Kim (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
https://doi.org/10.1016/j.jallcom.2016.02.067
22 K Pelle, M Wittmann, K Lovrics, Z Noszticzius (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
https://doi.org/10.1021/jp047472a
23 U Pinkernell, U Von Gunten (2001). Bromate minimization during ozonation: mechanistic considerations. Environmental Science & Technology, 35(12): 2525–2531
https://doi.org/10.1021/es001502f pmid: 11432558
24 M Sánchez-Polo, U von Gunten, J Rivera-Utrilla (2005). Efficiency of activated carbon to transform ozone into *OH radicals: Influence of operational parameters. Water Research, 39(14): 3189–3198
https://doi.org/10.1016/j.watres.2005.05.026 pmid: 16005933
25 D Shahidi, R Roy, A Azzouz (2015). Advances in catalytic oxidation of organic pollutants—Prospects for thorough mineralization by natural clay catalysts. Applied Catalysis B: Environmental, 174–175: 277–292
https://doi.org/10.1016/j.apcatb.2015.02.042
26 Z Song, M Wang, Z Wang, Y Wang, R Li, Y Zhang, C Liu, Y Liu, B Xu, F Qi (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
https://doi.org/10.1021/acs.est.9b01361 pmid: 30997803
27 Z Song, Y Zhang, C Liu, B Xu, F Qi, D Yuan, S Pu (2019b). Insight into OH and O2formation in heterogeneous catalytic ozonation by delocalized electrons and surface oxygen-containing functional groups in layered-structure nanocarbons. Chemical Engineering Journal, 357: 655–666
https://doi.org/10.1016/j.cej.2018.09.182
28 E Teixidó, E Piqué, J Gonzalez-Linares, J M Llobet, J Gómez-Catalán (2015). Developmental effects and genotoxicity of 10 water disinfection by-products in zebrafish. Journal of Water and Health, 13(1): 54–66
https://doi.org/10.2166/wh.2014.006 pmid: 25719465
29 J Vecchietti, M A Baltanás, C Gervais, S E Collins, G Blanco, O Matz, M Calatayud, A Bonivardi (2017). Insights on hydride formation over cerium-gallium mixed oxides: A mechanistic study for efficient H2 dissociation. Journal of Catalysis, 345: 258–269
https://doi.org/10.1016/j.jcat.2016.11.029
30 U von Gunten (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
https://doi.org/10.1016/S0043-1354(02)00458-X pmid: 12600375
31 Q Wang, Z Yang, J Ma, J Wang, L Wang, M Guo (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
https://doi.org/10.1080/19443994.2015.1079261
32 W Wang, Q Zhu, F Qin, Q Dai, X Wang (2018). Fe doped CeO2 nanosheets as Fenton-like heterogeneous catalysts for degradation of salicylic acid. Chemical Engineering Journal, 333: 226–239
https://doi.org/10.1016/j.cej.2017.08.065
33 Q Y Wu, Y T Zhou, W Li, X Zhang, Y Du, H Y Hu (2019). Underestimated risk from ozonation of wastewater containing bromide: Both organic byproducts and bromate contributed to the toxicity increase. Water Research, 162: 43–52
https://doi.org/10.1016/j.watres.2019.06.054 pmid: 31254885
34 Y Wu, C Wu, Y Wang, C Hu (2014). Inhibition of nano-metal oxides on bromate formation during ozonation process. Ozone Science and Engineering, 36(6): 549–559
https://doi.org/10.1080/01919512.2014.904735
35 W Xingyi, K Qian, L Dao (2009). Catalytic combustion of chlorobenzene over MnOx-CeO2 mixed oxide catalysts. Applied Catalysis B: Environmental, 86(3–4): 166–175
https://doi.org/10.1016/j.apcatb.2008.08.009
36 Z Xu, M Xie, Y Ben, J Shen, F Qi, Z Chen (2019). Efficiency and mechanism of atenolol decomposition in Co-FeOOH catalytic ozonation. Journal of Hazardous Materials, 365: 146–154
https://doi.org/10.1016/j.jhazmat.2018.11.006 pmid: 30419461
37 J Yang, H Zhang, Z Zhang, B Lai (2019). Degradation of 2,4-dinitrophenol in aqueous solution by microscale Fe0/H2O2/O3 process. Environmental Engineering Science, 36(2): 207–218
https://doi.org/10.1089/ees.2018.0143
38 Z Ye, H Tai, T Xie, Z Yuan, C Liu, Y Jiang (2016). Room temperature formaldehyde sensor with enhanced performance based on reduced graphene oxide/titanium dioxide. Sensors and Actuators. B, Chemical, 223: 149–156
https://doi.org/10.1016/j.snb.2015.09.102
39 T Zhang, W Chen, J Ma, Z Qiang (2008). Minimizing bromate formation with cerium dioxide during ozonation of bromide-containing water. Water Research, 42(14): 3651–3658
https://doi.org/10.1016/j.watres.2008.05.021 pmid: 18657284
40 L H Zhang, J Zhou, Z Q Liu, J B Guo (2019). Mesoporous CeO2 catalyst synthesized by using cellulose as template for the Ozonation of phenol. Ozone: Science and Engineering, 41(2): 166–174
[1] FSE-19095-OF-YB_suppl_1 Download
[1] Xiaoyan Guo, Chunyu Li, Chenghao Li, Tingting Wei, Lin Tong, Huaiqi Shao, Qixing Zhou, Lan Wang, Yuan Liao. G-CNTs/PVDF mixed matrix membranes with improved antifouling properties and filtration performance[J]. Front. Environ. Sci. Eng., 2019, 13(6): 81-.
[2] Zhichao Wu, Chang Zhang, Kaiming Peng, Qiaoying Wang, Zhiwei Wang. Hydrophilic/underwater superoleophobic graphene oxide membrane intercalated by TiO2 nanotubes for oil/water separation[J]. Front. Environ. Sci. Eng., 2018, 12(3): 15-.
[3] Tianyi Chen, Wancong Gu, Gen Li, Qiuying Wang, Peng Liang, Xiaoyuan Zhang, Xia Huang. Significant enhancement in catalytic ozonation efficacy: From granular to super-fine powdered activated carbon[J]. Front. Environ. Sci. Eng., 2018, 12(1): 6-.
[4] Fenghe Lv, Hua Wang, Zhangliang Li, Qi Zhang, Xuan Liu, Yan Su. Fabrication and photocatalytic ability of an Au/TiO2/reduced graphene oxide nanocomposite[J]. Front. Environ. Sci. Eng., 2018, 12(1): 4-.
[5] Shraddha Khamparia,Dipika Kaur Jaspal. Adsorption in combination with ozonation for the treatment of textile waste water: a critical review[J]. Front. Environ. Sci. Eng., 2017, 11(1): 8-.
[6] Yu YANG,Zhicheng YU,Takayuki NOSAKA,Kyle DOUDRICK,Kiril HRISTOVSKI,Pierre HERCKES,Paul WESTERHOFF. Interaction of carbonaceous nanomaterials with wastewater biomass[J]. Front. Environ. Sci. Eng., 2015, 9(5): 823-831.
[7] Jialu SHI,Shengnan YI,Chao LONG,Aimin LI. Effect of Fe loading quantity on reduction reactivity of nano zero-valent iron supported on chelating resin[J]. Front. Environ. Sci. Eng., 2015, 9(5): 840-849.
[8] Hong SUN,Min SUN,Yaobin ZHANG,Xie QUAN. Catalytic ozonation of reactive red X-3B in aqueous solution under low pressure: decolorization and OH· generation[J]. Front. Environ. Sci. Eng., 2015, 9(4): 591-595.
[9] Zhendong YANG, Aihua LV, Yulun NIE, Chun HU. Catalytic ozonation performance and surface property of supported Fe3O4 catalysts dispersions[J]. Front Envir Sci Eng, 2013, 7(3): 451-456.
[10] Yue PENG, Junhua LI. Ammonia adsorption on graphene and graphene oxide: a first-principles study[J]. Front Envir Sci Eng, 2013, 7(3): 403-411.
[11] Liqin JI, Xue BAI, Lincheng ZHOU, Hanchang SHI, Wei CHEN, Zulin HUA. One-pot preparation of graphene oxide magnetic nanocomposites for the removal of tetrabromobisphenol A[J]. Front Envir Sci Eng, 2013, 7(3): 442-450.
[12] LIU Zhengqian, MA Jun, ZHAO Lei. Effect of preparation parameters on catalytic properties of Pt/graphite[J]. Front.Environ.Sci.Eng., 2007, 1(4): 482-487.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed