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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.    2020, Vol. 14 Issue (6) : 102    https://doi.org/10.1007/s11783-020-1281-6
RESEARCH ARTICLE
Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer
Wenyue Li, Min Chen, Zhaoxiang Zhong, Ming Zhou(), Weihong Xing()
State Key Laboratory of Materials-Oriented Chemical Engineering, National Engineering Research Center for Specialized Separation Membranes, Nanjing Tech University, Nanjing 210009, China
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Abstract

• Cu2O NPs/H2O2 Fenton process was intensified by membrane dispersion.

• DMAc removal was enhanced to 98% for initial DMAc of 14000 mg/L.

• Analyzed time-resolved degradation pathway of DMAc under ·OH attack.

High-concentration industrial wastewater containing N,N-dimethylacetamide (DMAc) from polymeric membrane manufacturer was degraded in Cu2O NPs/H2O2 Fenton process. In the membrane-assisted Fenton process DMAc removal rate was up to 98% with 120 min which was increased by 23% over the batch reactor. It was found that ·OH quench time was extended by 20 min and the maximum ·OH productivity was notably 88.7% higher at 40 min. The degradation reaction rate constant was enhanced by 2.2 times with membrane dispersion (k = 0.0349 min1). DMAc initial concentration (C0) and H2O2 flux (Jp) had major influence on mass transfer and kinetics, meanwhile, membrane pore size (rp) and length (Lm) also affected the reaction rate. The intensified radical yield, fast mass transfer and nanoparticles high activity all contributed to improve pollutant degradation efficiency. Time-resolved DMAc degradation pathway was analyzed as hydroxylation, demethylation and oxidation leading to the final products of CO2, H2O and NO3 (rather than NH3 from biodegradation). Continuous process was operated in the dual-membrane configuration with in situ reaction and separation. After five cycling tests, DMAc removal was all above 95% for the initial [DMAc]0 = 14,000 mg/L in wastewater and stability of the catalyst and the membrane maintained well.

Keywords Ceramic membrane reactor      N,N-dimethylacetamide      Fenton process      Cu2O      Wastewater treatment     
Corresponding Author(s): Ming Zhou,Weihong Xing   
Issue Date: 12 June 2020
 Cite this article:   
Wenyue Li,Min Chen,Zhaoxiang Zhong, et al. Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer[J]. Front. Environ. Sci. Eng., 2020, 14(6): 102.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1281-6
https://academic.hep.com.cn/fese/EN/Y2020/V14/I6/102
Items Value
pH 7.6
DMAc 18000 mg/L
Ethylene glycol ~10 mg/L
Polyvinyl pyrrolidone <1 mg/L
COD 19080 mg/L
BOD5 718 mg/L
BOD5/COD 0.04
Total Nitrogen (TN) 2906 mg/L
Conductivity 0.443 mS/cm
Cl 23 mg/L
SO42 82 mg/L
Tab.1  Properties of the studied industrial wastewater
Fig.1  Cu2O NPs/H2O2 m-Fenton process with dual-membrane configuration (1-treated wastewater tank; 2-stirring; 3-membrane separation of Cu2O NPs; 4-membrane dispersion of H2O2; 5-pump and flowmeter; 6-H2O2 tank; 7-wastewater tank).
Fig.2  Tubular ceramic membrane assembled in m-Fenton reactor: (a) photograph, (b) cross-section SEM and (c) surface SEM images.
Fig.3  The as-prepared Cu2O nanocrystals: (a) XRD pattern and (b) SEM image.
Fig.4  Improved degradation efficiency with the m-Fenton process: (a) DMAc and (b) CODs removals ([DMAc]0 = 14,000 mg/L, [Cu2O] = 2.4 g/L, [H2O2] = 1.5 mol/L without membrane).
Fig.5  DMAc degradation in m-Fenton process with the effect of (a and b) initial concentration of DMAc (C0) and (c and d) membrane flux of H2O2 (Jp).
Fig.6  DMAc degradation in m-Fenton process with the effect from: (a?b) membrane mean pore size rp and (c?d) membrane length Lm ([DMAc]0 = 14000 mg/L, [Cu2O] = 2.4 g/L and [H2O2] = 1.5 mol/L without membrane).
Fig.7  
Fig.8  Intensified ·OH radical in m-Fenton process with ESR spectra analysis.
Fig.9  Degradation pathway of DMAc in the m-Fenton process analyzed with: (a) FTIR spectra, (b) total nitrogen analysis (c) GC-MS spectra.
Fig.10  Time-resolved degradation pathway of DMAc under ?OH radical attack.
Fig.11  Stability of m-Fenton process: a) cycling degradation tests on DMAc with Cu2O NPs/H2O2 m-Fenton process, b) XRD pattern and c) SEM image of Cu2O NPs before and after testing.
1 A Babuponnusami, K Muthukumar (2014). A review on Fenton and improvements to the Fenton process for wastewater treatment. Journal of Environmental Chemical Engineering, 2(1): 557–572
https://doi.org/10.1016/j.jece.2013.10.011
2 E Egidi, G Gasparini, R G Holdich, G T Vladisavljevic, S R Kosvintsev (2008). Membrane emulsification using membranes of regular pore spacing: droplet size and uniformity in the presence of surface shear. Journal of Membrane Science, 323: 414–420
https://doi.org/10.1016/j.memsci.2008.06.047
3 D Fan, L Ding, H Huang, M Chen, H Ren (2017). Fluidized-bed Fenton coupled with ceramic membrane separation for advanced treatment of flax wastewater. Journal of Hazardous Materials, 340: 390–398
https://doi.org/10.1016/j.jhazmat.2017.05.055
4 B Z Ge, J Zhang, P Lei, M Q Nie, P K Jin (2012). Study on degradation behavior of N,N-dimethylacetamide by photocatalytic oxidation in aqueous TiO2 suspensions. Desalination and Water Treatment, 42: 274–278
https://doi.org/10.5004/dwt.2012.3012
5 A R Ghazali, S H Inayat-Hussain (2014). N,N-dimethylacetamide. In: Encyclopedia of Toxicology. Wexler P, 3rd ed. Oxford: Academic Press, 594–597
6 R Guan, X Yuan, Z Wu, L Jiang, Y Li, G Zeng (2018). Principle and application of hydrogen peroxide based advanced oxidation processes in activated sludge treatment: A review. Chemical Engineering Journal, 339: 519–530
https://doi.org/10.1016/j.cej.2018.01.153
7 H Jiang, L Meng, R Chen, W Jin, W Xing, N Xu (2011). A novel dual-membrane reactor for continuous heterogeneous oxidation catalysis. Industrial & Engineering Chemistry Research, 50(18): 10458–10464
https://doi.org/10.1021/ie200398g
8 J M Burns, W J Cooper, J L Ferry, D W King, B P DiMento, K McNeill, C J Miller, W L Miller, B M Peake, S A Rusak, A L Rose, T D Waite (2012). Methods for reactive oxygen species (ROS) detection in aqueous environments. Aquatic Sciences, 74(4): 683–734
https://doi.org/10.1007/s00027-012-0251-x
9 G Kang, Y Cao (2014). Application and modification of poly(vinylidene fluoride) (PVDF)membranes: A review. Journal of Membrane Science, 463: 145–165
https://doi.org/10.1016/j.memsci.2014.03.055
10 L Kang, M Zhou, H Zhou, F Zhang, Z Zhong, W Xing (2019). Controlled synthesis of Cu2O microcrystals in membrane dispersion reactor and comparative activity in heterogeneous Fenton application. Powder Technology, 343: 847–854
https://doi.org/10.1016/j.powtec.2018.11.037
11 Y Lan, L Barthe, A Azais, C Gauss (2020). Feasibility of a heterogeneous Fenton membrane reactor containing a Fe-ZSM5 catalyst for pharmaceuticals degradation: Membrane fouling control and long-term stability. Separation and Purification Technology, 23(1): 115–920
12 H Li, R Cheng, Z Liu, C Du (2019). Waste control by waste: Fenton–like oxidation of phenol over Cu modified ZSM–5 from coal gangue. Science of the Total Environment, 68(3): 638–647
13 J Li, H Y Qi, Y P Shi (2009). Applications of titania and zirconia hollow fibers in sorptive micro-extraction of N,N-dimethylacetamide from water sample. Analytica Chimica Acta, 65(1): 182–187
14 X Li, S Chen, I Angelidaki, Y Zhang (2018). Bio-electro-Fenton processes for wastewater treatment: Advances and prospects. Chemical Engineering Journal, 35(4): 492–506
15 S Lu, N Wang, C Wang (2018). Oxidation and biotoxicity assessment of microcystin-LR using different AOPs based on UV, O3 and H2O2. Frontiers of Environmental Science & Engineering, 12(3): 12–21
https://doi.org/10.1007/s11783-018-1030-2
16 J Mao, X Quan, J Wang, C Gao, S Chen, H Yu, Y Zhang (2018). Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO3 perovskite for degradation of organic pollutants. Frontiers of Environmental Science & Engineering, 12(6): 10–18
https://doi.org/10.1007/s11783-018-1060-9
17 L Meng, H Guo, Z Dong, H Jiang, W Xing, W Jin (2013). Ceramic hollow fiber membrane distributor for heterogeneous catalysis: Effects of membrane structure and operating conditions. Chemical Engineering Journal, 223: 356–363
https://doi.org/10.1016/j.cej.2013.03.049
18 A N Pham, G Xing, C J Miller, T D Waite (2013). Fenton-like copper redox chemistry revisited: Hydrogen peroxide and superoxide mediation of copper-catalyzed oxidant production. Journal of Catalysis, 301: 54–64
https://doi.org/10.1016/j.jcat.2013.01.025
19 K V Plakas, A Mantza, S D Sklari, V T Zaspalis, A J Karabelas (2019). Heterogeneous Fenton-like oxidation of pharmaceutical diclofenac by a catalytic iron-oxide ceramic microfiltration membrane. Chemical Engineering Journal, 373: 700–708
https://doi.org/10.1016/j.cej.2019.05.092
20 B Prek, J Bezensek, M Kasunic, U Groselj, J Svete, B Stanovnik (2014). Reactions of enaminones and related compounds with N,N-dimethylacetamide dimethyl aceta: A simple one-pot metal-free synthesis of poly-substituted benzene derivatives. Tetrahedron, 70(14): 2359–2369
https://doi.org/10.1016/j.tet.2014.02.039
21 G Stefanos, L Siting, C Anna, R Sami, T A Masoud, M Bensimond, C Pulgarin (2017). Iron oxide-mediated semiconductor photo-catalysis vs. heterogeneous photo-Fenton treatment of viruses in wastewater: Impact of the oxide particle size. Journal of Hazardous Materials, 33(9): 223–231
22 J Tan, Y C Lu, J H Xu, G S Luo (2012). Mass transfer performance of gas–liquid segmented flow in micro-channels. Chemical Engineering Journal, 181–182: 229–235
https://doi.org/10.1016/j.cej.2011.11.067
23 J Tan, Y C Lu, J H Xu, G S Luo (2013). Modeling investigation of mass transfer of gas–liquid–liquid dispersion systems. Separation and Purification Technology, 108: 111–118
https://doi.org/10.1016/j.seppur.2013.01.010
24 J P Vítor, A M Pello, P M Joana, J Lee, M M Sandra, A R Rui (2020). Tube-in-tube membrane micro-reactor for photochemical UVC/H2O2 processes: A proof of concept. Chemical Engineering Journal, 37(9): 122–141
25 Z Xiong, B Lai, P Yang (2018). Insight into a highly efficient electrolysis-ozone process for N,N-dimethylacetamide degradation: Quantitative analysis of the role of catalytic ozonation, Fenton-like and peroxone reactions. Water Research, 140: 12–23
https://doi.org/10.1016/j.watres.2018.04.030
26 J H Xu, G S Luo, G G Chen, B Tan (2005). Mass transfer performance and two phase flow characteristic in membrane dispersion mini-extractor. Journal of Membrane Science, 249(1-2): 75–81
https://doi.org/10.1016/j.memsci.2004.09.039
27 F Zhang, G Dong, M Wang, Y Zeng, C Wang (2018a). Efficient removal of methyl orange using Cu2O as a dual function catalyst. Applied Surface Science, 444: 559–568
https://doi.org/10.1016/j.apsusc.2018.03.087
28 L Zhang, J Li, Z Chen, Y Tang, Y Yu (2006). Preparation of Fenton reagent with H2O2 generated by solar light-illuminated nano-Cu2O/MWNTs composites. Applied Catalysis A, General, 299: 292–297
https://doi.org/10.1016/j.apcata.2005.10.044
29 M Zhang, F Ji, Y Zhang, Z Pan, B Lai (2018b). Catalytic ozonation of N,N-dimethylacetamide (DMAc) in aqueous solution using nano-scaled magnetic CuFe2O4. Separation and Purification Technology, 193: 368–377
https://doi.org/10.1016/j.seppur.2017.10.028
30 Y Zhang, C He, V K Sharma, X Li, S Tian, Y Xiong (2011). A coupling process of membrane separation and heterogeneous Fenton-like catalytic oxidation for treatment of acid orange II-containing wastewater. Separation and Purification Technology, 80(1): 45–51
https://doi.org/10.1016/j.seppur.2011.04.004
31 H Zhou, L Kang, M Zhou, Z Zhong, W Xing (2018). Membrane enhanced COD degradation of pulp wastewater using Cu2O/H2O2 heterogeneous Fenton process. Chinese Journal of Chemical Engineering, 26(9): 1896–1903
https://doi.org/10.1016/j.cjche.2018.01.007
32 M Zhuo, O K Abass, K Zhang (2018). New insights into the treatment of real N,N-dimethylacetamide contaminated wastewater using a membrane bioreactor and its membrane fouling implications. RSC Advances, 8(23): 12799–12807
https://doi.org/10.1039/C8RA01657G
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