Abstract
This study aims to investigate the photocatalytic degradation performance, mechanism, and dynamics of methyl orange (MO) which is a widely used organic dye in textile industries as well a hazardous wastewater pollutant. The degradation process was catalyzed by employing a synthesized Fe3O4 magnetic nanoparticle (NP) using the coprecipitation method. The structural and morphological properties of the synthesized Fe3O4 NPs were investigated by employing XRD, HR-SEM, and XPS, which proved that acquired Fe3O4 NPs were in a pure phase. Moreover, the crystallite sizes fall in the range of 28–31.8 nm and were estimated by applying the Scherrer equation on the XRD spectrum as well as calculated independently by applying a statistical approach on the SEM micrographs. The UV–Vis maximum in the visible range at 468.8 nm consists of two absorption frequency bands due to the effect of the hydrogen-bond interaction between water and the azo nitrogens in the MO. A non-monotonic spectral dynamic accompanied by peak wavelength shifts, as well as the absolute signal amplitude and signal area of the MO band, suggests that a cleavage of the azo bond is not the only and/or the dominant process in the photocatalytic oxidization of the MO in a protic solvent. The overall absorbance process is a complicated response to a combination of nonspecific and specific solute-solvent interactions, dipole-dipole interactions, hydrogen-bonding networks, and other possible intermolecular interactions such as hydrophobic/hydrophilic interactions. A bi-exponential decay was found to be the best fitting function to model the decay of the time-dependent electrical conductivity of the MO aqueous solution under photocatalytic oxidization. The Fe3O4 NPs exhibited a 98.3% removal of MO within 110 min. Photocatalytic degradation of methyl orange can be modeled to the first-order model with a rate constant k of 0.037 min−1 taking into account the initial concentration of 1175 ppm of MO. The degradation/decolorization efficiency deduced from the low-frequency band of the visible spectra is around 99.4% after 110 min. The real-time degradation/decolorization efficiencies deduced from the overall absorbance maxima and the low-frequency band have a discrepancy of 50.1% at 20 min and 12.3% at 60 min representing the progressive attenuation of the H-bond impact dissociation of MO (degradation/decolorization).
Similar content being viewed by others
References
Ababneh, R., Telfah, A., Jum’h, I., Abudayah, M., Al-Abdallat, Y., Lambert, J., & Hergenröder, R. (2018). 1H NMR spectroscopy to investigate the kinetics and the mechanism of proton charge carriers ionization and transportation in hydrophilic/hydrophobic media: methyl sulfonic acid as a protonic ion source in water/alcohol binary mixtures. Journal of Molecular Liquids, 265, 621–628.
Alavi, S., Takeya, S., Ohmura, R., Woo, T. K., & Ripmeester, J. A. (2010). Hydrogen-bonding alcohol-water interactions in binary ethanol, 1-propanol, and 2 propanol+methane structure II clathrate hydrates. The Journal of Chemical Physics, 133.
Ali, A., Hira Zafar, M. Z., Ul Haq, I., Phull, A. R., Ali, J. S., & Hussain, A. (2016). Synthesis, characterization, applications, and challenges of iron oxide nanoparticles. Nanotechnology, Science and Applications, 9, 49.
Alinsafi, A., Evenou, F., Abdulkarim, E. M., Pons, M. N., Zahraa, O., Benhammou, A., Yaacoubi, A., & Nejmeddine, A. (2007). Treatment of textile industry wastewater by supported photocatalysis. Dyes and Pigments, 74, 439–445.
Alqaradawi, S., & Salman, S. (2002). Photocatalytic degradation of methyl orange as a model compound. Journal of Photochemistry and Photobiology A: Chemistry, 148, 161–168.
Andrade, A. L., Fabris, J., Ardisson, J., Valente, M. A., & Ferreira, J. M. F. (2012). Effect of tetramethylammonium hydroxide on nucleation, surface modification and growth of magnetic nanoparticles. Journal of Nanomaterials, 454, 759.
Bagbi, Y., Sarswat, A., Mohan, D., Pandey, A., & Solanki, P. R. (2017). Lead and chromium adsorption from water using L-cysteine functionalized magnetite (Fe3O4) nanoparticles. Scientific Reports, 7, 7672.
Barbosa, A., Bonifácio, L., & Dias, S. (2018). Wastewater reuse: case study of Abrunheira’s Industrial Water Treatment Plant, Modeling Innovation Sustainability and Technologies (pp. 311–317). Online ISBN 978–3–319-67,101-7.
Barreca, D., Carraro, G., Devi, A., Fois, E., Gasparotto, A., Seraglia, R., Maccato, C., Sada, C., Tabacchi, G., Tondello, E., Venzo, A., & Winter, M. (2012). β-Fe2O3 nanomaterials from an iron(II) diketonate-diamine complex: a study from molecular precursor to growth process. Dalton Transactions, 41, 149.
Bauer, M., Kauf, T., Christoffers, J., & Bertagnolli, H. (2005). Investigations into the metal species of the homogeneous iron(III) catalyzed Michael addition reaction. Physical Chemistry Chemical Physics, 7, 2664–2670.
Bureš, F. (2014). Fundamental aspects of property tuning in push–pull molecules. RSC Advances, 4, 58,826–58,851.
Carrazana, J., Reija, B., Ramos Cabrer, P., Al-Soufi, W., Novo, M., & Tato, J. V. (2004). Complexation of methyl orange with b-cyclodextrin: detailed analysis and application to quantification of polymer-bound cyclodextrin. Supramolecular Chemistry, 16, 549–559.
Chandler, D. (2005). Interfaces and the driving force of hydrophobic assembly. Nature, 437, 640–647.
Chiang, Y., & Lin, C. (2013). Powder Technology, 246, 137.
Chiha, M., Merouani, S., Hamdaoui, O., Baup, S., Gondrexon, N., & Pétrier, C. (2010). Ultrasonics Sonochemistry, 17, 773.
Cleland, W., & Kreevoy, M. (1994). Low-barrier hydrogen bonds an enzymic catalysis. Science, 264, 1887–1890.
Dagher, S., Soliman, A., Ziout, A., Tit, N., Hilal-Alnaqbi, A., Khashan, S., Alnaimat, F., & Qudeiri, J. (2018). Materials Research Express., 5, 065518.
Dannenberg, J. J. (2002). Cooperativity in hydrogen bonded aggregates. Models for crystals and peptides. Journal of Molecular Structure, 615, 219–226.
Eisenberg, D., & Kauzmann, W. (1969). The structure and properties of water. Oxford: Oxford University Press.
El Ghandoor, H., Zidan, H. M., Mostafa, M. H., & Khalil, M. I. M. I. (2012). Synthesis and some physical properties of magnetite (Fe3O4) nanoparticles. International Journal of Electrochemical Science, 7, 5734–5745.
Fujii, T., de Groot, F. M. F., Sawatzky, G. A., Voogt, F. C., Hibma, T., & Okada, K. (1999). Physical Review B: Condensed Matter and Materials Physics, 59, 3195.
Genuino, H., Mazrui, N., Seraji, M., Luo, Z., & Hoag, G. (2013). Green synthesis of iron nanomaterials for oxidative catalysis of organic environmental pollutants. In New and Future Developments in Catalysis. Catalysis for Remediation and Environmental Concerns (1st ed., pp. 41–61). Amsterdam: Elsevier.
Guerra, F. D., Campbell, M. L., Whitehead, D. C., & Alexis, F. (2017). Tunable properties of functional nanoparticles for efficient capture of VOCs. ChemistrySelect., 2, 9889–9894.
Guo, H., Stan, G., & Liu, Y. (2018). Soft Matter, 14, 1311.
Gutierrez, A. M., Dziubla, T. D., & Hilt, J. Z. (2017). Recent advances on iron oxide magnetic nanoparticles as sorbents of organic pollutants in water and wastewater treatment. Reviews on Environmental Health, 32, 111–117.
Handa, M., Miyamoto, H., Suzuki, T., Sawada, K., & Yukawa, Y. (1992). Solvent effects on acetylacetonato iron complexes. Inorganica Chimica Acta, 203, 61.
Heidari, A., Mir, N., & Nikkaran, A. R. (2016). Phenylalanine removal from water by Fe3O4 nanoparticles functionalized with two different surfactants. J Nanostructures, 6(3), 199–206.
Hibbert, F., & Emsley, J. (1990). Hydrogen bonding and chemical reactivity. Advances in Physical Organic Chemistry, 26, 255–379.
Ibrahim Dar, M., & Shivashankar, S. A. (2014). Single crystalline magnetite, maghemite, and hematite nanoparticles with rich coercivity. RSC Advances, 4, 4105.
Jang, S., Hira, S. A., Annas, D., Song, S., Yusuf, M., Park, J. C., Park, S., & Park, K. H. (2019). Recent novel hybrid Pd–Fe3O4 nanoparticles as catalysts for various C–C coupling reactions. Processes, 7, 422.
Jensen, M. Ø., Mouritsen, O. G., & Peters, G. H. (2004). The hydrophobic effect: molecular dynamics simulations of water confined between extended hydrophobic and hydrophilic surfaces. The Journal of Chemical Physics, 120, 9729–9744.
Jum’h, I., Abdelhay, A., Al-Taani, H., Telfah, A., Alnaief, M., & Rosiwal, S. (2017a). Fabrication and application of boron doped diamond BDD electrode in olive mill wastewater treatment in Jordan. Journal of Water Reuse and Desalination., 7, 502.
Jum’h, I., Telfah, A., Lambert, J., Gogiashvili, M., Al-Taani, H., & Hergenröder, R. (2017b). 13C and 1H NMR measurements to investigate the kinetics and the mechanism of acetic acid (CH3CO2H) ionization as a model for organic acid dissociation dynamics for polymeric membrane water filtration. Journal of Molecular Liquids, 227, 106–113.
Karimi, L., Zohoori, S., & Yazdanshenas, M. E. (2014). Photocatalytic degradation of azo dyes in aqueous solutions under UV irradiation using nano-strontium titanate as the nanophotocatalyst. Journal of Saudi Chemical Society, 18(5), 581–588.
Kreevoy, M. M., & Liang, T. M. (1980). Structures and isotopic fractionation factors of complexes, A1HA-2. Journal of the American Chemical Society, 102, 3315–3322.
Laage, D., & Hynes, J. T. (2006). Do more strongly hydrogen-bonded water molecules reorient more slowly. Chemical Physics Letters, 433, 80–85.
Lacroix, L.-M., Delpech, F., Nayral, C., Lachaize, S., & Chaudret, B. (2013). New generation of magnetic and luminescent nanoparticles for in vivo real-time imaging. Interface Focus, 3, 1–19.
Lau, Y. Y., Wong, Y. S., Teng, T. T., Morad, N., Rafatullah, M., & Ong, S. A. (2015). Degradation of cationic and anionic dyes in coagulation–flocculation process using bi-functionalized silica hybrid with aluminum-ferric as auxiliary agent. RSC Advances, 5, 34,206–34,215.
Legrini, O., Oliveros, E., & Braun, A. (1993). Photochemical processes for water treatment. Chemical Reviews, 93, 671.
Li, X., Zhang, Z., & Henrich, V. E. (1993). Inelastic electron background function for ultraviolet photoelectron spectra. Journal of Electron Spectroscopy and Related Phenomena, 63, 253–265.
Liland, K., Almøy, T., & Mevik, B.-H. (2010). Optimal choice of baseline correction for multivariate calibration of spectra. Applied Spectroscopy, 64, 1007–1016.
Lopez, J., González, F., Bonilla, F., Zambrano, G., & Gómez, M. (2010). RevistaLatinoamericana de Metalurgia y Materiales., 30, 60.
Lops, C., Ancona, A., Di Cesare, K., Dumontel, B., Garino, N., Canavese, G., Hérnandez, S., & Cauda, V. (2019). Sonophotocatalytic degradation mechanisms of rhodamine B dye via radicals generation by micro- and nano-particles of ZnO. Applied Catalysis. B, Environmental, 243, 629–640.
Mascolo, M. C., Pei, Y., & Ring, T. A. (2013). Room temperature co-precipitation synthesis of magnetite nanoparticles in a large pH window with different bases. Materials (Basel)., 6, 5549–5567.
Mortazavian, S., Saber, A., & James, D. E. (2019). Optimization of photocatalytic degradation of acid blue 113 dye and acid red 88 textile dyes in UV-C/TiO2 suspension system: application of response surface methodology (RSM). Catal, 9, 1–19.
Namanga, J., Foba, J., Ndinteh, D. T., Yufanyi, D. M., & Krause, R. W. M. (2013, 2013). Synthesis and magnetic properties of a superparamagnetic nanocomposite “Pectin-Magnetite Nanocomposite”. Journal of Nanomaterials, 137275, 8 pages.
Nançoz, C., Licari, G., Beckwith, J. S., Soederberg, M., Dereka, B., Rosspeintner, A., Yushchenko, O., Letrun, R., Richert, S., Lang, B., & Vauthey, E. (2018). Physical Chemistry Chemical Physics, 20, 7254–7264.
Nardo, L., Paderno, R., Andreoni, A., Másson, M., Haukvik, T., & Tønnesen, H. H. (2008). Role of H-bond formation in the photoreactivity of curcumin. Spectroscopy, 22, 187–198.
Özen, A. S., Doruker, P., & Aviyente, V. (2007). Effect of cooperative hydrogen bonding in azo−hydrazone tautomerism of azo dyes. The Journal of Physical Chemistry A, 111, 51 13,506–13,514.
Pacheco-Álvarez, M., Rodríguez-Narváez, O., Wrobel, K., Navarro-Mendoza, R., Nava-Montes de Oca, J., & Peralta-Hernández, J. (2018a). Improvement of the Degradation of Methyl Orange Using a TiO2/BDD Composite Electrode to Promote Electrochemical and Photoelectro-Oxidation Processes. Int. J. Electrochem. Sci., 13, 11549–11567.
Pacheco-Álvarez, M., Rodríguez-Narváez, O., Wrobel, K., Navarro-Mendoza, R., Nava-Montes de Oca, J., & Peralta-Hernández, J. (2018b). International Journal of Electrochemical Science, 13, 11,549.
Park, H., Ayala, P., Deshusses, M., Mulchandani, A., Choi, H., & Myung, N. (2008). Electrodeposition of maghemite (γ-Fe2O3) nanoparticles. Chemical Engineering Journal, 139, 208.
Reeves, R. L., Kaiser, R. S., Maggio, M. S., Sylvestre, E. A., & Lawton, W. H. (1973). Analysis of the visual spectrum of methyl orange in solvents and in hydrophobic binding sites. Canadian Journal of Chemistry, 51(4), 628–635.
Reichardt, C. (1994). Solvatochromic dyes as solvent polarity indicators. Chemical Reviews, 94, 2319–2358.
Revers, R. L., & Kaiser, R. S. (1972). In H. H. G. Jel-linek (Ed.), Water structure at the water-polymer interface (p. 56). New York: Plenum Press.
Rizzo, L., Malato, S., Antakyali, D., Beretsou, V. G., Đolić, M. B., Gernjak, W., Heath, E., Ivancev-Tumbas, I., Karaolia, P., & Ribeiro, A. R. L. (2019). Consolidated vs new advanced treatment methods for the removal of contaminants of emerging concern from urban wastewater. Science of the Total Environment, 655, 986–1008.
Ruzza, P., Hussain, R., Biondi, B., Calderan, A., Tessari, I., Bubacco, L., & Siligardi, G. (2015). Effects of trehalose on thermodynamic properties of alpha-synuclein revealed through synchrotron radiation circular dichroism. Biomolecules, 5, 724–734.
Sauer, T., Neto, G., Jose, H., & Moreira, R. (2002). Journal of Photochemistry and Photobiology A: Chemistry, 149, 147.
Silva, A., Santos, L. H. M. L. M., Antão, C., Delerue-Matos, C., & Figueiredo, S. A. (2017). Ecotoxicological evaluation of chemical indicator substances present as micropollutants in laboratory wastewaters. Global NEST Journal, 19, 94–99.
Sun, S., & Zheng, H. (2002). Size-controlled synthesis of magnetite nanoparticles. Journal of the American Chemical Society, 124, 8204–8205.
Tzitzi, M., Vayenas, D. V., & Lyberatos, G. (1994). Pretreatment of textile industry wastewaters with ozone. Water Science and Technology, 29, 151–160.
Wu, S., Sun, A., Zhai, F., Wang, J., Xu, W., Zhang, Q., & Volinsky, A. (2011). Fe3O4 magnetic nanoparticles synthesis from tailings by ultrasonic chemical co-precipitation. Materials Letters, 651, 882.
Xin, X., Wei, Q., Yang, B. J., Yan, L., Feng, R., Chen, G., Du, B., & Li, H. (2012). Highly efficient removal of heavy metal ions by amine-functionalized mesoporous Fe3O4 nanoparticles. Chemical Engineering Journal, 184, 132–140.
Yaseen, D. A., & Scholz, M. (2019). Textile dye wastewater characteristics and constituents of synthetic effluents: a critical review. International Journal of Environmental Science and Technology, 16, 1193.
Zysler, R., Mansilla, M., & Fiorani, D. (2004). Surface effects in α-Fe2O3 nanoparticles. The European Physical Journal B-Condensed Matter and Complex Systems, 41, 171.
Acknowledgments
The authors would like to acknowledge the national program “Faculty for Factory” (FFF) in the University of Jordan for initiation the links with industrial sector in Jordan. The scientific and the financial support of the Deanship of Scientific Research at the German Jordanian University (Project number SNRE 2/2013) is gratefully appreciated. A sincere acknowledgement goes to the Max Planck Institute, Erlangen-Germany for granting us access to their XPS spectrometer and to the technological assistance that was offered in the characterizations.
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Al-Abdallat, Y., Jum’h, I., Al Bsoul, A. et al. Photocatalytic Degradation Dynamics of Methyl Orange Using Coprecipitation Synthesized Fe3O4 Nanoparticles. Water Air Soil Pollut 230, 277 (2019). https://doi.org/10.1007/s11270-019-4310-y
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-019-4310-y