Hydroxyl radical intensified Cu₂O NPs/H₂O₂ process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer

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.

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 notably 88.7% 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 (J_p) had major influence on mass transfer and kinetics, meanwhile, membrane pore size (r_p) and length (L_m) 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.

Graphical abstract

Keywords

Ceramic membrane reactor / N,N-dimethylacetamide / Fenton process / Cu₂O / Wastewater treatment

References

[1] 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

[2] 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

[3] 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

[4] 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

[5] Ghazali A R, Inayat-Hussain S H (2014). N,N-dimethylacetamide. In: Encyclopedia of Toxicology. Wexler P, 3rd ed. Oxford: Academic Press, 594–597

[6] 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

[7] Jiang H, Meng L, Chen R, Jin W, Xing W, Xu N (2011). A novel dual-membrane reactor for continuous heterogeneous oxidation catalysis. Industrial & Engineering Chemistry Research, 50(18): 10458–10464

[8] 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

[9] Kang G, Cao Y (2014). Application and modification of poly(vinylidene fluoride) (PVDF)membranes: A review. Journal of Membrane Science, 463: 145–165

[10] 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

[11] 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

[12] 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

[13] 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

[14] 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

[15] 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

[16] 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

[17] 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

[18] 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

[19] 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

[20] 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

[21] 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

[22] 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

[23] 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

[24] 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

[25] 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

[26] 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

[27] 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

[28] 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

[29] 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

[30] 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

[31] 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

[32] 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).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-020-1281-6 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2020 Higher Education Press