New Sustainable Approach for the Production of Fe3O4/Graphene Oxide-Activated Persulfate System for Dye Removal in Real Wastewater

MDPI AG - Tập 12 Số 3 - Trang 733
Md. Nahid Pervez1,2,3, Wei He3, Tiziano Zarra2, Vincenzo Naddeo2, Yaping Zhao3
1Department of Textile Engineering, Southeast University, Tejgaon, Dhaka-1208, Bangladesh
2Sanitary Environmental Engineering Division (SEED), Department of Civil Engineering, University of Salerno, Via Giovanni Paolo II 132, 84084, Fisciano, SA, Italy
3School of Ecological and Environmental Science, Shanghai Key Laboratory for Urban Ecological Process and Eco-Restoration, East China Normal University, Shanghai 200241, China

Tóm tắt

Persulfate (PS)-activated, iron-based heterogeneous catalysts have attracted significant attention as a potential advanced and sustainable water purification system. Herein, a novel Fe3O4 impregnated graphene oxide (Fe3O4@GO)-activated persulfate system (Fe3O4@GO+K2S2O8) was synthesized by following a sustainable protocol and was tested on real wastewater containing dye pollutants. In the presence of the PS-activated system, the degradation efficiency of Rhodamine B (RhB) was significantly increased to a level of ≈95% compared with that of Fe3O4 (≈25%). The influences of different operational parameters, including solution pH, persulfate dosage, and RhB concentration, were systemically evaluated. This system maintained its catalytic activity and durability with a negligible amount of iron leached during successive recirculation experiments. The degradation intermediates were further identified through reactive oxygen species (ROS) studies, where surface-bound SO4− was found to be dominant radical for RhB degradation. Moreover, the degradation mechanism of RhB in the Fe3O4@GO+K2S2O8 system was discussed. Finally, the results indicate that the persulfate-activated Fe3O4@GO catalyst provided an effective pathway for the degradation of dye pollutants in real wastewater treatment.

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Tài liệu tham khảo

Contreras, M., Grande-Tovar, C.D., Vallejo, W., and Chaves-López, C. (2019). Bio-Removal of Methylene Blue from Aqueous Solution by Galactomyces geotrichum KL20A. Water, 11.

Pervez, M.N., and Stylios, G.K. (2018). Investigating the synthesis and characterization of a novel “green” H2O2-assisted, water-soluble chitosan/polyvinyl alcohol nanofiber for environmental end uses. Nanomaterials, 8.

Park, J.H., Shin, D.S., and Lee, J.K. (2019). Treatment of High-Strength Animal Industrial Wastewater Using Photo-Assisted Fenton Oxidation Coupled to Photocatalytic Technology. Water, 11.

Cuartero, 2019, Pulsed light for a cleaner dyeing industry: azo dye degradation by an advanced oxidation process driven by pulsed light, J. Clean. Prod., 217, 757, 10.1016/j.jclepro.2019.01.230

Hou, 2020, Persulfate activation induced by ascorbic acid for efficient organic pollutants oxidation, Chem. Eng. J., 382, 122355, 10.1016/j.cej.2019.122355

Liu, 2020, Cu (II)-enhanced degradation of acid orange 7 by Fe (II)-activated persulfate with hydroxylamine over a wide pH range, Chemosphere, 238, 124533, 10.1016/j.chemosphere.2019.124533

Pervez, M.N., Telegin, F.Y., Cai, Y., Xia, D., Zarra, T., and Naddeo, V. (2019). Efficient Degradation of Mordant Blue 9 Using the Fenton-Activated Persulfate System. Water, 11.

Zhang, 2019, Catalytic degradation of estrogen by persulfate activated with iron-doped graphitic biochar: Process variables effects and matrix effects, Chem. Eng. J., 378, 122141, 10.1016/j.cej.2019.122141

Deng, 2016, Heterogeneous degradation of orange II with peroxymonosulfate activated by ordered mesoporous MnFe2O4, Sep. Purif. Technol., 167, 181, 10.1016/j.seppur.2016.04.035

Wang, 2014, Magnetic Fe3O4/carbon sphere/cobalt composites for catalytic oxidation of phenol solutions with sulfate radicals, Chem. Eng. J., 245, 1, 10.1016/j.cej.2014.02.013

Yu, 2019, Iron-based metal-organic frameworks as novel platforms for catalytic ozonation of organic pollutant: Efficiency and mechanism, J. Hazard. Mater., 367, 456, 10.1016/j.jhazmat.2018.12.108

Liu, 2018, Treatment of landfill leachate biochemical effluent using the nano-Fe3O4/Na2S2O8 system: Oxidation performance, wastewater spectral analysis, and activator characterization, J. Environ. Manag., 208, 159, 10.1016/j.jenvman.2017.12.023

Peng, 2018, Adsorption and catalytic oxidation of pharmaceuticals by nitrogen-doped reduced graphene oxide/Fe3O4 nanocomposite, Chem. Eng. J., 341, 361, 10.1016/j.cej.2018.02.064

Kang, 2019, Nickel in hierarchically structured nitrogen-doped graphene for robust and promoted degradation of antibiotics, J. Clean. Prod., 218, 202, 10.1016/j.jclepro.2019.01.323

Yan, 2017, Determination of trace rhodamine B by spectrofluorometry and magnetic solid phase extraction based on a 3D reduced graphene oxide composite, Anal. Methods., 9, 5433, 10.1039/C7AY01622K

Yao, 2014, Magnetic recoverable MnFe2O4 and MnFe2O4-graphene hybrid as heterogeneous catalysts of peroxymonosulfate activation for efficient degradation of aqueous organic pollutants, J. Hazard. Mater., 270, 61, 10.1016/j.jhazmat.2014.01.027

Tran, 2017, Graphene oxide/Fe3O4/chitosan nanocomposite: A recoverable and recyclable adsorbent for organic dyes removal. application to methylene blue, Mater. Res. Express., 4, 035701, 10.1088/2053-1591/aa6096

Ojha, 2017, Photo-Fenton degradation of organic pollutants using a zinc oxide decorated iron oxide/reduced graphene oxide nanocomposite, Ceram. Int., 43, 1290, 10.1016/j.ceramint.2016.10.079

Gong, 2016, Degradation of dye wastewater by persulfate activated with Fe3O4/graphene nanocomposite, J. Water Reuse Desalin., 6, 553, 10.2166/wrd.2016.187

Jain, 2007, Removal of the hazardous dye rhodamine B through photocatalytic and adsorption treatments, J. Environ. Manag., 85, 956, 10.1016/j.jenvman.2006.11.002

Hummers, 1958, Preparation of graphitic oxide, J. Am. Chem. Soc., 80, 1339, 10.1021/ja01539a017

Sellers, 1980, Spectrophotometric determination of hydrogen peroxide using potassium titanium(IV) oxalate, Analyst, 105, 950, 10.1039/an9800500950

Kim, 2015, Heterogeneous catalytic oxidation of as(iii) on nonferrous metal oxides in the presence of H2O2, Environ. Sci. Technol., 49, 3506, 10.1021/es5056897

Czili, 2008, Applicability of coumarin for detecting and measuring hydroxyl radicals generated by photoexcitation of TiO2 nanoparticles, Appl. Catal. B-Environ., 81, 295, 10.1016/j.apcatb.2008.01.001

Rabani, 1965, The pulse radiolysis of aqueous tetranitromethane. 1 i. rate constants and the extinction coefficient of eaq-. Ii. oxygenated solutions, J. Phys. Chem., 69, 53, 10.1021/j100885a011

Yang, 2015, Rapid degradation of methylene blue in a novel heterogeneous Fe3O4@ rGO@ TiO2-catalyzed photo-Fenton system, Sci. Rep., 5, 10632, 10.1038/srep10632

Gan, 2018, The fabrication of bio-renewable and recyclable cellulose based carbon microspheres incorporated by CoFe2O4 and the photocatalytic properties, J. Clean. Prod., 196, 594, 10.1016/j.jclepro.2018.06.086

Romero, 2010, Diuron abatement using activated persulphate: Effect of pH, Fe (II) and oxidant dosage, Chem. Eng. J., 162, 257, 10.1016/j.cej.2010.05.044

Liang, 2007, Influence of pH on persulfate oxidation of TCE at ambient temperatures, Chemosphere, 66, 106, 10.1016/j.chemosphere.2006.05.026

Xu, 2020, Reduced graphene oxide-supported metal organic framework as a synergistic catalyst for enhanced performance on persulfate induced degradation of trichlorophenol, Chemosphere, 240, 124849, 10.1016/j.chemosphere.2019.124849

Yan, 2011, Degradation of sulfamonomethoxine with Fe3O4 magnetic nanoparticles as heterogeneous activator of persulfate, J. Hazard. Mater., 186, 1398, 10.1016/j.jhazmat.2010.12.017

Gong, 2015, An effective heterogeneous iron-based catalyst to activate peroxymonosulfate for organic contaminants removal, Chem. Eng. J., 267, 102, 10.1016/j.cej.2015.01.010

Zhao, 2018, Co-Mn layered double hydroxide as an effective heterogeneous catalyst for degradation of organic dyes by activation of peroxymonosulfate, Chemosphere, 204, 11, 10.1016/j.chemosphere.2018.04.023

Ahmadi, 2019, The application of thermally activated persulfate for degradation of acid blue 92 in aqueous solution, Int. J. Ind. Chem., 10, 1, 10.1007/s40090-019-0188-1

Liang, 2004, Persulfate oxidation for in situ remediation of TCE. II. activated by chelated ferrous ion, Chemosphere., 55, 1225, 10.1016/j.chemosphere.2004.01.030

Chen, 2017, Heterogeneously catalyzed persulfate by CuMgFe layered double oxide for the degradation of phenol, Appl. Catal. A-Gen., 538, 19, 10.1016/j.apcata.2017.03.020

Bendjama, 2019, Using photoactivated acetone for the degradation of chlorazol black in aqueous solutions: Impact of mineral and organic additives, Sci. Total. Environ., 653, 833, 10.1016/j.scitotenv.2018.11.007

Dong, 2019, Oxidation of bisphenol A by persulfate via Fe3O4-α-MnO2 nanoflower-like catalyst: Mechanism and efficiency, Chem. Eng. J., 357, 337, 10.1016/j.cej.2018.09.179

Yan, 2016, Degradation of trichloroethylene by activated persulfate using a reduced graphene oxide supported magnetite nanoparticle, Chem. Eng. J., 295, 309, 10.1016/j.cej.2016.01.085

Lv, 2018, Modulation of valence band maximum edge and photocatalytic activity of BiOX by incorporation of halides, Chemosphere, 191, 427, 10.1016/j.chemosphere.2017.09.149

Fang, 2013, Superoxide radical driving the activation of persulfate by magnetite nanoparticles: Implications for the degradation of PCBs, Appl. Catal. B-Environ., 129, 325, 10.1016/j.apcatb.2012.09.042

Cheng, 2017, Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes, Water. Res., 113, 80, 10.1016/j.watres.2017.02.016

Wang, 2015, Nitrogen-doped reduced graphene oxide as a bifunctional material for removing bisphenols: Synergistic effect between adsorption and catalysis, Environ. Sci. Technol., 49, 6855, 10.1021/acs.est.5b01059

Tang, 2018, Enhanced activation process of persulfate by mesoporous carbon for degradation of aqueous organic pollutants: Electron transfer mechanism, Appl. Catal. B Environ., 231, 1, 10.1016/j.apcatb.2018.02.059

Zhu, 2019, Growth of graphene-supported hollow cobalt sulfide nanocrystals via MOF-templated ligand exchange as surface-bound radical sinks for highly efficient bisphenol A degradation, Appl. Catal. B-Environ., 242, 238, 10.1016/j.apcatb.2018.09.088

Wang, 2018, Heterogeneous activation of peroxymonosulfate by hierarchical CuBi2O4 to generate reactive oxygen species for refractory organic compounds degradation: Morphology and surface chemistry derived reaction and its mechanism, Environ. Sci. Pollut. Res., 25, 4419, 10.1007/s11356-017-0773-9

2017, Structure and optical properties of Fe3O4 nanoparticles synthesized by co-precipitation method with different organic modifiers, Mater. Charact., 131, 148, 10.1016/j.matchar.2017.06.034

Zhu, 2018, Efficient activation of persulfate by Fe3O4@ β-cyclodextrin nanocomposite for removal of bisphenol A, RSC Adv., 8, 14879, 10.1039/C8RA01696H

Gao, 2016, Insights into the mechanism of heterogeneous activation of persulfate with a clay/iron-based catalyst under visible LED light irradiation, Appl. Catal. B-Environ., 185, 22, 10.1016/j.apcatb.2015.12.002

Jiang, J., Zhang, D., Zhang, H., Yu, K., Li, N., and Zheng, G. (2019). Degradation mechanism study of fluoroquinolones in UV/Fe2+/peroxydisulfate by on-line mass spectrometry. Chemosphere.