Abstract
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 notably88.7% higher at 40 min. The degradation reaction rate constant was enhanced by 2.2 times with membrane dispersion (k = 0.0349 min−1). 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.
Similar content being viewed by others
References
Babuponnusami A, Muthukumar K (2014). A review on Fenton and improvements to the Fenton process for wastewater treatment. Journal of Environmental Chemical Engineering, 2(1): 557–572
Egidi E, Gasparini G, Holdich R G, Vladisavljevic G T, Kosvintsev S R (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
Fan D, Ding L, Huang H, Chen M, Ren H (2017). Fluidized-bed Fenton coupled with ceramic membrane separation for advanced treatment of flax wastewater. Journal of Hazardous Materials, 340: 390–398
Ge B Z, Zhang J, Lei P, Nie M Q, Jin P K (2012). Study on degradation behavior of N, N-dimethylacetamide by photocatalytic oxidation in aqueous TiO2 suspensions. Desalination and Water Treatment, 42: 274–278
Ghazali A R, Inayat-Hussain S H (2014). N, N-dimethylacetamide. In: Encyclopedia of Toxicology. Wexler P, 3rd ed. Oxford: Academic Press, 594–597
Guan R, Yuan X, Wu Z, Jiang L, Li Y, Zeng G (2018). Principle and application of hydrogen peroxide based advanced oxidation processes in activated sludge treatment: A review. Chemical Engineering Journal, 339: 519–530
Jiang H, Meng L, Chen R, Jin W, Xing W, Xu N (2011). A novel dualmembrane reactor for continuous heterogeneous oxidation catalysis. Industrial & Engineering Chemistry Research, 50(18): 10458–10464
Burns J M, Cooper W J, Ferry J L, King D W, DiMento B P, McNeill K, Miller C J, Miller W L, Peake B M, Rusak S A, Rose A L, Waite T D (2012). Methods for reactive oxygen species (ROS) detection in aqueous environments. Aquatic Sciences, 74(4): 683–734
Kang G, Cao Y (2014). Application and modification of poly(vinylidene fluoride) (PVDF)membranes: A review. Journal of Membrane Science, 463: 145–165
Kang L, Zhou M, Zhou H, Zhang F, Zhong Z, Xing W (2019). Controlled synthesis of Cu2O microcrystals in membrane dispersion reactor and comparative activity in heterogeneous Fenton application. Powder Technology, 343: 847–854
Lan Y, Barthe L, Azais A, Gauss C (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
Li H, Cheng R, Liu Z, Du C (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
Li J, Qi H Y, Shi Y P (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
Li X, Chen S, Angelidaki I, Zhang Y (2018). Bio-electro-Fenton processes for wastewater treatment: Advances and prospects. Chemical Engineering Journal, 35(4): 492–506
Lu S, Wang N, Wang C (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
Mao J, Quan X, Wang J, Gao C, Chen S, Yu H, Zhang Y (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
Meng L, Guo H, Dong Z, Jiang H, Xing W, Jin W (2013). Ceramic hollow fiber membrane distributor for heterogeneous catalysis: Effects of membrane structure and operating conditions. Chemical Engineering Journal, 223: 356–363
Pham A N, Xing G, Miller C J, Waite T D (2013). Fenton-like copper redox chemistry revisited: Hydrogen peroxide and superoxide mediation of copper-catalyzed oxidant production. Journal of Catalysis, 301: 54–64
Plakas K V, Mantza A, Sklari S D, Zaspalis V T, Karabelas A J (2019). Heterogeneous Fenton-like oxidation of pharmaceutical diclofenac by a catalytic iron-oxide ceramic microfiltration membrane. Chemical Engineering Journal, 373: 700–708
Prek B, Bezensek J, Kasunic M, Groselj U, Svete J, Stanovnik B (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
Stefanos G, Siting L, Anna C, Sami R, Masoud T A, Bensimond M, Pulgarin C (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
Tan J, Lu Y C, Xu J H, Luo G S (2012). Mass transfer performance of gas-liquid segmented flow in micro-channels. Chemical Engineering Journal, 181–182: 229–235
Tan J, Lu Y C, Xu J H, Luo G S (2013). Modeling investigation of mass transfer of gas-liquid-liquid dispersion systems. Separation and Purification Technology, 108: 111–118
Vítor J P, Pello A M, Joana P M, Lee J, Sandra M M, Rui A R (2020). Tube-in-tube membrane micro-reactor for photochemical UVC/H2O2 processes: A proof of concept. Chemical Engineering Journal, 37(9): 122–141
Xiong Z, Lai B, Yang P (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
Xu J H, Luo G S, Chen G G, Tan B (2005). Mass transfer performance and two phase flow characteristic in membrane dispersion mini-extractor. Journal of Membrane Science, 249(1–2): 75–81
Zhang F, Dong G, Wang M, Zeng Y, Wang C (2018a). Efficient removal of methyl orange using Cu2O as a dual function catalyst. Applied Surface Science, 444: 559–568
Zhang L, Li J, Chen Z, Tang Y, Yu Y (2006). Preparation of Fenton reagent with H2O2 generated by solar light-illuminated nano-Cu2O/MWNTs composites. Applied Catalysis A, General, 299: 292–297
Zhang M, Ji F, Zhang Y, Pan Z, Lai B (2018b). Catalytic ozonation of N, N-dimethylacetamide (DMAc) in aqueous solution using nano-scaled magnetic CuFe2O4. Separation and Purification Technology, 193: 368–377
Zhang Y, He C, Sharma V K, Li X, Tian S, Xiong Y (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
Zhou H, Kang L, Zhou M, Zhong Z, Xing W (2018). Membrane enhanced COD degradation of pulp wastewater using Cu2O/H2O2 heterogeneous Fenton process. Chinese Journal of Chemical Engineering, 26(9): 1896–1903
Zhuo M, Abass O K, Zhang K (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
Acknowledgements
The authors would like to acknowledge the financial support from National Natural Science Foundation of China (Grant No. 21921006).
Author information
Authors and Affiliations
Corresponding authors
Additional information
Highlights
• 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.
Electronic supplementary material
Rights and permissions
About this article
Cite this article
Li, W., Chen, M., Zhong, Z. et al. Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer. Front. Environ. Sci. Eng. 14, 102 (2020). https://doi.org/10.1007/s11783-020-1281-6
Received:
Revised:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11783-020-1281-6