Water Science and Engineering 2020, 13(4) 286-298 DOI:   https://doi.org/10.1016/j.wse.2020.12.001  ISSN: 1674-2370 CN: 32-1785/TV

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Green synthesis
Iron nanoparticles
Azo dye
Fenton-like process

Green synthesis of bentonite-supported iron nanoparticles as a heterogeneous Fenton-like catalyst: Kinetics of decolorization of reactive blue 238 dye

Ahmed Khudhair Hassan a, *, Ghayda Yaseen Al-Kindi b, Dalal Ghanim b

a Environment and Water Directorate, Ministry of Science and Technology, Baghdad 10070, Iraq
b Sanitary and Environmental Branch, Civil Engineering Department, University of Technology, Baghdad 10009, Iraq


This study aimed to synthesize green tea nano zero-valent iron (GT-NZVI) and bentonite-supported green tea nano zero-valent iron (B-GT-NZVI) nanoparticles using green tea extracts in an environmentally sustainable way. Bentonite was used as a support material because it disperses and stabilizes GT-NZVI, and it helps to reduce the cost, increase the adsorption capacity of GT-NZVI, and decrease the optimum amount of GT-NZVI used in Fenton-like oxidation. A scanning electron microscope, atomic force microscopy, and a Fourier transform infrared spectroscope were used to characterize GT-NZVI and B-GT-NZVI, while the zeta potential was measured to evaluate the stability of iron nanoparticles. The decolorization kinetics of reactive blue 238 (RB 238) dye in the aqueous phase in the Fenton-like oxidation process were investigated as well. The effects of various experimental conditions such as reaction time, dosages of catalysts, concentration of H2O2, temperature, addition of inorganic salts, and other parameters were investigated. The results show that the oxidative degradation efficiencies of RB 238 dye catalyzed by GT-NZVI and B-GT-NZVI were 93.5% and 96.2%, respectively, at the optimum reaction conditions as follows: c(H2O2) = 5 mmol/L, ρ(GT-NZVI) or ρ(B-GT-NZVI) = 0.5 g/L, c(RB 238 dye) = 0.05 mmol/L, and pH = 2.5 at 180 min. The best catalytic performance was exhibited when B-GT-NZVI was used. Three kinetic models were employed, and the second-order model was found to be the best model representing the experimental kinetic data of RB 238 dye. The value of activation energy decreased from 38.22 kJ/mol for GT-NZVI to 14.13 kJ/mol for B-GT-NZVI. This indicates that the effect of B-GT-NZVI in decreasing the energy barrier is more pronounced than that of the GT-NZVI catalyst, leading to improved Fenton-like oxidation processes.

Keywords Green synthesis   Iron nanoparticles   Azo dye   Fenton-like process   Kinetics  
Received 2020-03-25 Revised 2020-08-18 Online: 2020-12-30 
DOI: https://doi.org/10.1016/j.wse.2020.12.001
Corresponding Authors: Ahmed Khudhair Hassan
Email: ahmedkhh71@yahoo.com
About author:


Abdel-Aziz, H.M., Farag, R.S., Abdel-Gawad, S.A., 2019. Carbamazepine removal from aqueous solution by green synthesis zero-valent iron/Cu nanoparticles with Ficus Benjamina leaves’ extract. International Journal of Environmental Research. 13(5), 843-852. https://doi.org/10.1007/s41742-019-00220-w.

Ali, I., Peng, C.S., Khan, Z.M., Sultan, M., Naz, I., Ali, M., Farid, H.U., Mahmood, M.H., Ahsen, R., 2019. Removal of crystal violet and eriochrome black T dyes from aqueous solutions by magnetic nanoparticles biosynthesized from leaf extract of Fraxinus Chinensis Roxb. Polish Journal of Environmental Studies. 28(4), 2027-2040. https://doi.org/10.15244/pjoes/89505.

Bao, T., Jin, J., Damtie, M.M., Wu, K., Yu, Z.M., Wang, L., Chen, J., Zhang, Y., Frost, R.L., 2019. Green synthesis and application of nanoscale zero-valent iron/rectorite composite material for P-chlorophenol degradation via heterogeneous Fenton reaction. Journal of Saudi Chemical Society. 23(7), 864-878. https://doi.org/10.1016/j.jscs.2019.02.001.

Beheshtkhoo, N., Kouhbanani, M.A.J., Savardashtaki, A., Amani, A.M., Taghizadeh, S., 2018. Green synthesis of iron oxide nanoparticles by aqueous leaf extract of Daphne mezereum as a novel dye removing material. Applied Physics A. 124(5), 363. https://doi.org/10.1007/s00339-018-1782-3.

Brantut, N., Heap, M.J., Meredith, P.G., Baud, P., 2013. Time-dependent cracking and brittle creep in crustal rocks: A review. Journal of Structural Geology. 52, 17-43. https://doi.org/10.1016/j.jsg.2013.03.007.

Chi, Z.X., Wang, Z., Chu, H.Q., Bin, P., Lucian, L., 2017. Bentonite-supported nanoscale zero-valent iron granulated electrodes for industrial wastewater remediation. RSC Advances. 7(70), 44605-44613. https://doi.org/10.1039/C7RA07584G.

Demirezen, D.A., Y?ld?z, Y.S., Y?lmaz, D.D., 2019. Amoxicillin degradation using green synthesized iron oxide nanoparticles: Kinetics and mechanism analysis. Environmental Nanotechnology, Monitoring & Management. 11, 100219. https://doi.org/10.1016/j.enmm.2019.100219.

Ebrahiminezhad, A., Taghizadeh, S., Ghasemi, Y., Berenjian, A., 2018. Green synthesized nanoclusters of ultra-small zero valent iron nanoparticles as a novel dye removing material. Science of the Total Environment. 621, 1527-1532.  https://doi.org/10.1016/j.scitotenv.2017.10.076.

Elmoubarki, R., Mahjoubi, F.Z., Tounsadi, H., Moustadraf, J., Abdennouri, M., Zouhri, A., ElAlbani, A., Barka, N., 2015. Adsorption of textile dyes on raw and decanted Moroccan clays: Kinetics, equilibrium and thermodynamics. Water Resources and Industry. 9, 16–29. https://doi.org/10.1016/j.wri.2014.11.001.

Fida, H., Guo, S., Zhang, G.K., 2015. Preparation and characterization of bifunctional Ti-Fe kaolinite composite for Cr(VI) removal. Journal of Colloid and Interface Science. 442, 30-38. https://doi.org/10.1016/j.jcis.2014.11.023.

Gudelj, I., Hrenovi?, J., Dragi?evi?, T.L., Delaš, F., Soljan, V., Gudelj, H., 2011. Azo dyes, their environmental effects, and defining a strategy for their biodegradation and detoxification. Archives of Industrial Hygiene and Toxicology. 62(1), 91-101. https://doi.org/10.2478/10004-1254-62-2011-2063.

Gwenzi, W., Chaukura, N., 2018. Organic contaminants in African aquatic systems: Current knowledge, health risks, and future research directions. Science of the Total Environment. 619–620, 1493-1514. https://doi.org/10.1016/j.scitotenv.2017.11.121.

Hashemian, S., 2013. Fenton-like oxidation of malachite green solutions: Kinetic and thermodynamic study. Journal of Chemistry, 2013, 1-7. http://dx.doi.org/10.1155/2013/809318.

Hassan, A.K., Rahman, M.M., Chattopadhay, G., Naidu, R., 2019. Kinetic of the degradation of sulfanilic acid azochromotrop (SPADNS) by Fenton process coupled with ultrasonic irradiation or L-cysteine acceleration. Environmental Technology & Innovation. 15, 100380. https://doi.org/10.1016/j.eti.2019.100380.

Herlekar, M., Barve, S., Kumar, R., 2014. Plant-mediated green synthesis of iron nanoparticles. Journal of Nanoparticles. 2014, 140614. https://doi.org/10.1155/2014/140614.

Huang, L.L., Weng, X.L., Chen, Z.L., Meghara, M., Naidu, R., 2014. Green synthesis of iron nanoparticles by various tea extracts: Comparative study of the reactivity. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy. 130, 295-301. https://doi.org/10.1016/j.saa.2014.04.037.

Kerkez, D.V., Tomaševi?, D.D., Kozma, G., Be?eli?-Tomin, M.R., Prica, M.D., Ron?evi?, S.D., Kukovecz, A.,C., Dalmacija, B.D., Kónya, Z., 2014. Three different clay-supported nanoscale zero-valent iron materials for industrial azo dye degradation: A comparative study. Journal of the Taiwan Institute of Chemical Engineers. 45(5), 2451-2461. https://doi.org/10.1016/j.jtice.2014.04.019.

Kiruba Daniel, S.C.G., Vinothini, G., Subramanian, N., Nehru, K., Sivakumar, M., 2013. Biosynthesis of Cu, ZVI, and Ag nanoparticles using Dodonaea viscosa extract for antibacterial activity against human pathogens. Journal of Nanoparticle Research. 15(1), 1319. https://doi.org/10.1007/s11051-012-1319-1.

Lellis, B., Fávaro-Polonio, C.Z., Pamphile, J.A., Polonio, J.C., 2019. Effects of textile dyes on health and the environment and bioremediation potential of living organisms. Biotechnology Research and Innovation, 3(2), 275-290. https://doi.org/10.1016/j.biori.2019.09.001.

Machado, S., Pacheco, J.G., Nouws, H.P.A., Albergaria, J.T., Delerue-Matos, C., 2015. Characterization of green zero-valent iron nanoparticles produced with tree leaf extracts. Science of The Total Environment. 533, 76-81. https://doi.org/10.1016/j.scitotenv.2015.06.091.

Mahmoud, A.S., Farag, R.S., Elshfai, M.M., 2020. Reduction of organic matter from municipal wastewater at low cost using green synthesis nano iron extracted from black tea: Artificial intelligence with regression analysis. Egyptian Journal of Petroleum, 29(1), 9-20. https://doi.org/10.1016/j.ejpe.2019.09.001.

Melnyk, A., Kuklińska, K., Wolska, L., Namie?nik, J., 2014. Chemical pollution and toxicity of water samples from stream receiving leachate from controlled municipal solid waste (MSW) landfill. Environmental Research. 135, 253-261. https://doi.org/10.1016/j.envres.2014.09.010.

Nicodemos Ramos, M.D., Sousa, L.A., Aguiar, A., 2020. Effect of cysteine using Fenton processes on decolorizing different dyes: A kinetic study. Environmental Technology, 1-26. https://doi.org/10.1080/09593330.2020.1776402.

Önal, E.S., Yatkin, T., Ergüt, M., Özer, A., 2017. Green synthesis of iron nanoparticles by aqueous extract of Eriobotrya japonica leaves as a heterogeneous Fenton-like catalyst: Degradation of basic red 46. International Journal of Chemical Engineering and Applications, 8(5), 327-333. https://doi.org/10.18178/ijcea.2017.8.5.678 .

Paz, A., Carballo, J., Pérez, M.J., Domínguez, J.M., 2017. Biological treatment of model dyes and textile wastewaters. Chemosphere. 181, 168-177. https://doi.org/10.1016/j.chemosphere.2017.04.046.

Satapanajaru, T., Chompuchan, C., Suntornchot, P., Pengthamkeerati, P., 2011. Enhancing decolorization of reactive black 5 and reactive red 198 during nano zerovalent iron treatment. Desalination. 266(1-3), 218-230. https://doi.org/10.1016/j.desal.2010.08.030.

Serrano-Martínez, A., Mercader-Ros, M.T., Martínez-Alcalá, I., Lucas-Abellán, C., Gabaldón, J.A., Gómez-López, V.M., 2020. Degradation and toxicity evaluation of azo dye Direct red 83:1 by an advanced oxidation process driven by pulsed light. Journal of Water Process Engineering, 37, 101530. https://doi.org/10.1016/j.jwpe.2020.101530.

Setia, H., Gupta, R., Wanchoo, R.K., 2013. Stability of nanofluids. Materials Science Forum. 757, 139-149. https://doi.org/10.4028/www.scientific.net/MSF.757.139.

Shahwan, T., Sirriah, S.A., Nairat, M., Boyac?, E., Ero?lu, A.E., Scott, T.B., Hallam, K.R., 2011. Green synthesis of iron nanoparticles and their application as a Fenton-like catalyst for the degradation of aqueous cationic and anionic dyes. Chemical Engineering Journal, 172(1), 258-266. https://doi.org/10.1016/j.cej.2011.05.103.

Shao, J.C., Yu, X.N., Zhou, M., Cai, X.Q., Yu, C., 2018. Nanoscale zero-valent iron decorated on bentonite/graphene oxide for removal of copper ions from aqueous solution. Materials. 11(6), 945. https://doi.org/10.3390/ma11060945.

Shih, Y.-H., Tso, C.-P., 2012. Fast decolorization of azo-dye congo red with zerovalent iron nanoparticles and sequential mineralization with a Fenton reaction. Environmental Engineering Science. 29(10), 929-933. https://doi.org/10.1089/ees.2010.0433.

Shukla, A.K., Iravani, S., 2018. Green Synthesis, Characterization and Applications of Nanoparticles. 1st ed. Elsevier.

Singh, J., Dutta, T., Kim, K.H., Rawat, M., Samddar, P., Kumar, P., 2018. Green synthesis of metals and their oxide nanoparticles: Applications for environmental remediation. Journal of Nanobiotechnology. 16(1), 84. https://doi.org/10.1186/s12951-018-0408-4.

Sravanthi, K., Ayodhya, D., Swamy, P.Y., 2019. Green synthesis, characterization and catalytic activity of 4-nitrophenol reduction and formation of benzimidazoles using bentonite supported zero valent iron nanoparticles. Materials Science for Energy Technologies. 2(2), 298-307. https://doi.org/10.1016/j.mset.2019.02.003.

Trovó, A.G., Hassan, A.K., Sillanpää, M., Tang, W.Z., 2016. Degradation of Acid Blue 161 by Fenton and photo-Fenton processes. International Journal of Environmental Science and Technology. 13(1), 147-158. https://doi.org/10.1007/s13762-015-0854-6.

Vilardi, G., Parisi, M., Verdone, N., 2019a. Simultaneous aggregation and oxidation of nZVI in Rushton equipped agitated vessel: Experimental and modelling. Powder Technology, 353, 238-246. https://doi.org/10.1016/j.powtec.2019.05.033.

Vilardi, G., Stoller, M., Di Palma, L., Boodhoo, K., Verdone, N., 2019b. Metallic iron nanoparticles intensified production by spinning disk reactor: Optimization and fluid dynamics modelling. Chemical Engineering and Processing-Process Intensification, 146, 107683. https://doi.org/10.1016/j.cep.2019.107683.

Wang, F.Y., Yang, W.W., Zheng, F.Y., Sun, Y.H., 2018. Removal of Cr (VI) from simulated and leachate wastewaters by Bentonite-supported zero-valent iron nanoparticles. International Journal of Environmental Research and Public Health. 15(10), 2162. https://doi.org/10.3390/ijerph15102162.

Wang, H., Chen, L., Weng, L.L., Zhang, M.Y., Shen, Q., 2014a. Surface properties and dissolution kinetics of tea polyphenols. Journal of Adhesion Science and Technology. 28(24), 2416-2423. https://doi.org/10.1080/01694243.2014.968420.

Wang, Q.C., Liu, S.G., Gao, H.P., 2019.Treatment of hydroxyquinone-containing wastewater using precipitation method with barium salt. Water Science and Engineering. 12(1), 55-61. https://doi.org/10.1016/j.wse.2019.03.003.

Wang, T., Lin, J.J., Chen, Z.L., Megharaj, M., Naidu, R., 2014b. Green synthesized iron nanoparticles by green tea and eucalyptus leaves extracts used for removal of nitrate in aqueous solution. Journal of Cleaner Production. 83, 413-419. https://doi.org/10.1016/j.jclepro.2014.07.006.

Weng, X.L., Owens, G., Chen, Z.L., 2020. Synergetic adsorption and Fenton-like oxidation for simultaneous removal of ofloxacin and enrofloxacin using green synthesized Fe NPs. Chemical Engineering Journal, 382, 122871. https://doi.org/10.1016/j.cej.2019.122871.

Wu, Y., Zeng, S.L., Wang, F.F., Megharaj, M., Naidu, R., Chen, Z.L., 2015. Heterogeneous Fenton-like oxidation of malachite green by iron-based nanoparticles synthesized by tea extract as a catalyst. Separation and Purification Technology. 154, 161-167. https://doi.org/10.1016/j.seppur.2015.09.022.

Yuan, M., Fu, X.X., Yu, J., Xu, Y., Huang, J.L., Li, Q.B., Sun, D.H., 2020. Green synthesized iron nanoparticles as highly efficient Fenton-like catalyst for degradation of dyes. Chemosphere, 261, 127618. https://doi.org/10.1016/j.chemosphere.2020.127618.

Zahrim, A.Y., Hilal, N., 2013.Treatment of highly concentrated dye solution by coagulation/flocculation-sand filtration and nanofiltration. Water Resources and Industry. 3, 23-34. https://doi.org/10.1016/j.wri.2013.06.001.

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