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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2015, Vol. 9 Issue (4) : 615-624     https://doi.org/10.1007/s11783-014-0706-5
RESEARCH ARTICLE |
Catalytic ozonation of organic compounds in water over the catalyst of RuO2/ZrO2-CeO2
Jianbing WANG1,*(),Guoqing WANG1,Chunli YANG1,Shaoxia YANG2,Qing HUANG1
1. School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, China
2. School of Energy and Power Engineering, North China Electric Power University, Beijing 102206, China
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Abstract

This research investigates the performances of RuO2/ZrO2-CeO2 in catalytic ozonation for water treatment. The results show that RuO2/ZrO2-CeO2 was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO2/Al2O3 and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO2/ZrO2-CeO2 did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO2/ZrO2-CeO2 played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO2/ZrO2-CeO2, the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO2/ZrO2-CeO2 in catalytic ozonation for water treatment.

Keywords ozonation      ruthenium      oxalic acid      dimethyl phthalate      disinfection byproduct     
Corresponding Authors: Jianbing WANG   
Online First Date: 07 May 2014    Issue Date: 25 June 2015
 Cite this article:   
Jianbing WANG,Guoqing WANG,Chunli YANG, et al. Catalytic ozonation of organic compounds in water over the catalyst of RuO2/ZrO2-CeO2[J]. Front. Environ. Sci. Eng., 2015, 9(4): 615-624.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-014-0706-5
http://journal.hep.com.cn/fese/EN/Y2015/V9/I4/615
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Jianbing WANG
Guoqing WANG
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Shaoxia YANG
Qing HUANG
Fig.1  XRD patterns of RuO2/ZrO2-CeO2 (a) and ZrO2-CeO2 (b)
Fig.2  Removals of oxalic acid in semi-batch (a) and dynamic (b) catalytic ozonation experiments
Fig.3  Removal of oxalic acid in the catalytic ozonation with different Ru loading
Fig.4  Removals of DMP (a) and TOC (b) in catalytic ozonation of DMP in water
samples total removal ozonation adsorption catalysis
value/(mg·L-1) ratio/% value/(mg·L-1) contribution/% value/(mg·L-1) contribution/% value/(mg·L-1) contribution/%
ZrO2-CeO2 2.01 65 0.62 31 1.01 50 0.39 19
RuO2/ZrO2-CeO2 2.47 80 0.62 25 1.11 45 0.74 30
Tab.1  Contributions of ozonation, adsorption and catalysis to the overall TOC removal
No. sampling site TOC/(mg·L-1) UV254 conductivity/(μs·cm-1) pH
mean std. dev. mean std. dev. mean std. dev. mean std. dev.
1 Qiaoxin Town 2.32 0.198 0.043 0.0073 339 28.5 7.7 0.42
2 Beishicao Town 2.25 0.157 0.043 0.0068 338 26.5 7.6 0.40
3 Xingshou Town 2.38 0.234 0.048 0.0039 329 25.8 8.1 0.35
4 Nanshao Town 2.50 0.224 0.046 0.0051 336 25.6 8.5 0.31
5 Machi Kou 2.47 0.225 0.048 0.0053 330 25.2 8.3 0.35
6 Yangfan Town 2.52 0.209 0.047 0.0046 327 24.2 8.2 0.31
7 Hotspring Town 2.45 0.228 0.048 0.0054 311 29.5 8.2 0.34
8 Blue-dragon Bridge 2.50 0.233 0.044 0.0049 308 25.9 8.1 0.28
9 Huoqiying Bridge 2.29 0.183 0.045 0.0050 310 29.5 7.7 0.40
10 Changchun Bridge 2.33 0.205 0.043 0.0036 301 23.6 7.4 0.24
11 Yuyuan Pond 3.20 0.278 0.064 0.0082 368 35.7 7.3 0.22
Tab.2  Common water quality parameters for the natural water samples
samples MCAA/(μg·L-1) MBAA/(μg·L-1) DCAA/(μg·L-1) TCAA/(μg·L-1) BCAA/(μg·L-1) BDCAA/(μg·L-1) HAAFP/(μg·L-1) THMFP/(μg·L-1)
mean std. dev. mean std. dev. mean std. dev. mean std. dev. mean std. dev. mean std. dev.
1 6.0 0.55 26.0 3.51 0.1 0.01 51.0 4.80 1.1 0.13 6.9 0.68 91.1 149.3
2 7.5 0.61 28.5 2.15 0.1 0.01 53.0 8.25 1.3 0.12 6.6 0.69 97.0 145.5
3 7.3 0.64 27.1 2.60 0.1 0.01 51.1 4.17 0.7 0.08 6.3 0.55 92.6 160.7
4 7.0 0.69 26.5 3.65 0.1 0.01 51.8 4.22 0.6 0.08 6.2 0.51 92.2 156.4
5 7.5 0.63 26.7 1.75 0.2 0.01 52.3 4.48 0.7 0.08 6.3 0.57 93.7 163.7
6 8.3 0.67 28.0 5.00 0.1 0.02 53.7 4.30 0.8 0.10 6.4 0.59 97.3 163.0
7 7.2 0.68 27.0 2.83 0.4 0.05 58.9 7.40 1.5 0.14 6.3 0.67 101.3 160.2
8 6.8 0.58 26.5 2.34 0.3 0.03 56.3 6.12 1.6 0.23 6.3 0.63 97.8 165.8
9 6.3 0.54 25.0 3.83 0.1 0.02 55.4 5.68 1.5 0.20 6.1 0.51 94.4 152.4
10 6.8 0.68 25.3 2.74 0.3 0.02 57.1 5.80 1.7 0.14 6.1 0.55 97.3 150.1
11 27.0 3.56 30.2 2.97 0.1 0.01 76.1 6.32 2.0 0.16 7.1 0.64 142.5 220.0
Tab.3  Concentrations of haloacetic acids, HAAFPs and THMFPs of the natural water samples
Fig.5  Reductions of HAAsFP (a), TCAAFP (b) and THMFP (c) in adsorption, noncatalytic ozonation and catalytic ozonation processes
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