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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.    2021, Vol. 15 Issue (4) : 78    https://doi.org/10.1007/s11783-020-1371-5
RESEARCH ARTICLE
Optimization of the O3/H2O2 process with response surface methodology for pretreatment of mother liquor of gas field wastewater
Haoran Feng, Min Liu, Wei Zeng, Ying Chen()
College of Architecture and Environment, Sichuan University, Chengdu 610065, China
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Abstract

• Real ML-GFW with high salinity and high organics was degraded by O3/H2O2 process.

• Successful optimization of operation conditions was attained using RSM based on CCD.

• Single-factor experiments in advance ensured optimal experimental conditions.

• The satisfactory removal efficiency of TOC was achieved in spite of high salinity.

• The initial pH plays the most significant role in the degradation of ML-GFW.

The present study reports the use of the O3/H2O2 process in the pretreatment of the mother liquor of gas field wastewater (ML-GFW), obtained from the multi-effect distillation treatment of the gas field wastewater. The range of optimal operation conditions was obtained by single-factor experiments. Response surface methodology (RSM) based on the central composite design (CCD) was used for the optimization procedure. A regression model with Total organic carbon (TOC) removal efficiency as the response value was established (R2 = 0.9865). The three key factors were arranged according to their significance as: pH>H2O2 dosage>ozone flow rate. The model predicted that the best operation conditions could be obtained at a pH of 10.9, an ozone flow rate of 0.8 L/min, and H2O2 dosage of 6.2 mL. The dosing ratio of ozone was calculated to be 9.84 mg O3/mg TOC. The maximum removal efficiency predicted was 75.9%, while the measured value was 72.3%. The relative deviation was found to be in an acceptable range. The ozone utilization and free radical quenching experiments showed that the addition of H2O2 promoted the decomposition of ozone to produce hydroxyl radicals (·OH). This also improved the ozone utilization efficiency. Gas chromatography-mass spectrometry (GC-MS) analysis showed that most of the organic matters in ML-GFW were degraded, while some residuals needed further treatment. This study provided the data and the necessary technical supports for further research on the treatment of ML-GFW.

Keywords High salinity      High organic matters      Gas field wastewater      O3/H2O2      Response surface methodology     
Corresponding Author(s): Ying Chen   
Just Accepted Date: 29 October 2020   Issue Date: 02 December 2020
 Cite this article:   
Haoran Feng,Min Liu,Wei Zeng, et al. Optimization of the O3/H2O2 process with response surface methodology for pretreatment of mother liquor of gas field wastewater[J]. Front. Environ. Sci. Eng., 2021, 15(4): 78.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1371-5
https://academic.hep.com.cn/fese/EN/Y2021/V15/I4/78
Fig.1  Schematic representation of the O3/H2O2 system.
Fig.2  The effects of (a) reaction time (pH= 9.7, ozone flow rate= 1 L/min, H2O2 dosage= 4 mL), (b) pH (reaction time= 180 min, ozone flow rate= 1 L/min, H2O2 dosage= 4 mL), (c) ozone flow rate (reaction time= 180 min, pH= 9.7, H2O2 dosage= 4 mL), (d) H2O2 dosage (reaction time= 180 min, pH= 9.7, ozone flow rate= 0.8 L/min) on TOC removal.
Factors Levels
–α –1 0 +1
pH 6.64 8.00 10.00 12.00 13.36
Ozone flow rate (L/min) 0.46 0.60 0.80 1.00 1.14
H2O2 dosage (mL) 2.64 4.00 6.00 8.00 9.36
Tab.1  Factors and levels of RSM experiment (CCD)
Run Factors Y: TOC removal
(%)
A: pH B: Ozone flow rate(L/min) C: H2O2 dosage (mL)
1 6.64 0.80 6.00 31.2
2 8.00 0.60 8.00 38.9
3 8.00 1.00 4.00 39.3
4 8.00 0.60 4.00 39.2
5 8.00 1.00 8.00 47.9
6 10.00 0.46 6.00 56.0
7 10.00 0.80 6.00 74.2
8 10.00 0.80 6.00 75.9
9 10.00 0.80 6.00 72.3
10 10.00 0.80 2.64 49.2
11 10.00 0.80 9.36 57.2
12 10.00 0.80 6.00 72.7
13 10.00 0.80 6.00 74.0
14 10.00 0.80 6.00 72.1
15 10.00 1.14 6.00 64.2
16 12.00 1.00 8.00 61.5
17 12.00 1.00 4.00 60.5
18 12.00 0.60 8.00 63.3
19 12.00 0.60 4.00 62.4
20 13.36 0.80 6.00 59.1
Tab.2  The response of TOC removal efficiency of optimization experiments
Source Sum of Squares df a) Mean Square F-Value p-Value Prob>F
Model 3480.38 9 386.71 81.29 <0.0001
A 1224.73 1 1224.73 257.44 <0.0001
B 27.14 1 27.14 5.71 0.0380
C 40.96 1 40.96 8.61 0.0149
AB 20.48 1 20.48 4.30 0.0648
AC 5.12 1 5.12 1.08 0.3240
BC 10.13 1 10.13 2.13 0.1753
A2 1451.32 1 1451.32 305.07 <0.0001
B2 322.23 1 322.23 67.73 <0.0001
C2 744.82 1 744.82 156.56 <0.0001
Residual 47.57 10 4.76
Lack of Fit 37.04 5 7.41 3.52 0.0969
Pure Error 10.53 5 2.11
Tab.3  ANOVA of the RSM model
Fig.3  Plots of RSM results ((a), (b)) and 3D response surface of combine effect of A-B ((c), (d)), B-C ((e), (f)), A-C ((g), (h)) on TOC removal efficiency.
Fig.4  Plots of mechanism verification experiments under optimized conditions (reaction time= 180 min, pH= 10.9, ozone flow rate= 0.8 L/min, H2O2 dosage= 6.2 mL): (a) the ozone utilization rate with O3/H2O2 and single ozone process, (b) effect of TBA on TOC removal efficiency (TBA dosage= 15 mmol/L).
Fig.5  Results of analysis of organic compounds by GC-MS.
Fig.6  Possible degradation pathways of main contaminants.
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