Synthesis of 32 Layered Reduced Graphene Oxide Nanosheet with Carbon-Defects via of Sono-Solvothermal Route for Removal of Ciprofloxacin from Water, Study of Kinetics and Adsorption Isotherm

Document Type : Research Article

Authors

Reactor and Catalyst Research Center, Faculty of Chemical Engineering, Sahand University of Technology, Sahand New Town, Tabriz, I.R. IRAN

Abstract

In this research, 32 layered reduced graphene oxide (rGO) nanosheets with carbon-defects, as a nano-adsorbent, were designed through the one-pot sono-solvothermal method. The properties of this nano-adsorbent were determined using various analyses such as XRD, Raman, FESEM, 3D analysis, TEM, EDS, FTIR and UV-Vis spectroscopy analyses. The results revealed that rGO nanosheets well formed during sono-solvothermal process due to the efficient reduction of graphene oxide. So that, according to the results of Raman analysis, the reduction of GO to rGO as well as the creation of structural defects were confirmed. Besides, in view of the UV-Vis upshots, it was observed that a shoulder peak around 300 nm of graphene oxide spectrum, belong to the electrons transition from n to π* of C=O band which is existed in the functional groups, was disappeared in the rGO spectrum. This nano-adsorbent was evaluated in the elimination of the ciprofloxacin (fluoroquinolone antibiotic) as a model pollutant of emerging contaminants category. On the basis of experimental outcomes, the maximum adsorption efficiency of ciprofloxacin antibiotic was obtained by rGO (98.9%) during 120 min. Moreover, the study of adsorption isotherms showed that the adsorption process is consistent with the Friendlich adsorption isotherm. 

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[1] Perreault F., De Faria A.F., Elimelech M., Environmental Applications of Graphene-Based Nanomaterials, Chemical Society Reviews, 44(16): 5861-5896 (2015).
[2] Kemp K.C., Seema H., Saleh M., Le N.H., Mahesh K., Chandra V., Kim K.S., Environmental Applications Using Graphene Composites: Water Remediation and Gas Adsorption, Nanoscale, 5(8): 3149-3171 (2013).
[3] پازکی م.، قاسم زاده ر.، یاوری م.، عبدلی م.ع.، بررسی عملکرد نانوذره تیتانیوم دی‌اکسید نقره دوپ (2Ag/TiO) در تخریب فوتوکاتالیستی اریترومایسین، نشریه شیمی و مهندسی شیمی ایران، 37(1): 72-63 (1397).
 [4] Yosefi L., Haghighi M., Allahyari S., Solvothermal Synthesis of Flowerlike p-BiOI/n-ZnFe2O4 with Enhanced Visible Light Driven Nanophotocatalyst Used in Removal of Acid Orange 7 from Wastewater, Separation and Purification Technology, 178: 18-28 (2017).
[5] Maleki M., Haghighi M., Sono-Dispersion of CuS-CdS over TiO2 in One-Pot Hydrothermal Reactor as Visible-Light-Driven Nanostructured Photocatalyst, Journal of Molecular Catalysis A: Chemical, 424: 283-296 (2016).
[7] Hama Aziz K.H., Miessner H., Mueller S., Kalass D., Moeller D., Khorshid I., Rashid M.A.M., Degradation of Pharmaceutical Diclofenac and Ibuprofen in Aqueous Solution, a Direct Comparison of Ozonation, Photocatalysis, and Non-Thermal Plasma, Chemical Engineering Journal, 313: 1033-1041 (2017).
[8] Gad-Allah T.A., Ali M.E.M., Badawy M.I., Photocatalytic Oxidation of Ciprofloxacin Under Simulated Sunlight, Journal of Hazardous Materials, 186(1): 751-755 (2011).
[9] Yang X., Chen Z., Zhao W., Liu C., Qian X., Zhang M., Wei G., Khan E., Hau Ng Y., Sik Ok Y., Recent Advances in Photodegradation of Antibiotic Residues in Water, Chemical Engineering Journal, 405: 126806 (2021).
[11] Zandipak R., Sobhanardakani S., Novel Mesoporous Fe3O4/SiO2/CTAB–SiO2 as an Effective Adsorbent for the Removal of Amoxicillin and Tetracycline from Water, Clean Technologies and Environmental Policy, 20(4): 871-885 (2018).
[12] Ghoochian M., Panahi H.A., Sobhanardakani S., Taghavi L., Hassani A.H., Synthesis and Application of Fe3O4/SiO2/Thermosensitive/PAMAM-CS Nanoparticles as a Novel Adsorbent for Removal of Tamoxifen from Water Samples, Microchemical Journal, 145: 1231-1240 (2019).
[13] Rodríguez E.M., Márquez G., Tena M., Álvarez P.M., Beltrán F.J., Determination of Main Species Involved in the First Steps of TiO2 Photocatalytic Degradation of Organics with the Use of Scavengers: the Case of Ofloxacin, Applied Catalysis B: Environmental, 178: 44-53 (2015).
[14] Olatunde O.C., Onwudiwe D.C., Graphene-Based Composites as Catalysts for the Degradation of Pharmaceuticals, International Journal of Environmental Research and Public Health, 18(4): 1529 (2021).
[16] Yan Y., Sun S., Song Y., Yan X., Guan W., Liu X., Shi W., Microwave-Assisted in Situ Synthesis of Reduced Graphene Oxide-BiVO4 Composite Photocatalysts and Their Enhanced Photocatalytic Performance for the Degradation of Ciprofloxacin, Journal of hazardous materials, 250: 106-114 (2013).
[17] Van Wieren E.M., Seymour M.D., Peterson J.W., Interaction of the Fluoroquinolone Antibiotic, Ofloxacin, with Titanium Oxide Nanoparticles in Water: ADSORPTION and Breakdown, Science of The Total Environment, 441: 1-9 (2012).
[19] Zandipak R., Sobhan Ardakani S., Shirzadi A., Synthesis and Application of Nanocomposite Fe3O4@SiO2@CTAB–SiO2 as a Novel Adsorbent for Removal of Cyclophosphamide from Water Samples, Separation Science and Technology, 55(3): 456-470 (2020).
[20] Sobhan Ardakani S., Cheraghi M., Jafari A., Zandipak R., PECVD Synthesis of ZnO/Si thin film as a Novel Adsorbent for Removal of Azithromycin from Water Samples, International Journal of Environmental Analytical Chemistry: 1-18 (2020).
[21] Cheraghi M., Lorestani B., Zandipak R., Sobhanardakani S., GO@Fe3O4@ZnO@CS Nanocomposite as a Novel Adsorbent for Removal of Doxorubicin Hydrochloride from Aqueous Solutions, Toxin Reviews, 41(1): 82-91 (2022).
[23] Wang H., Li J., Huo P., Yan Y., Guan Q., Preparation of Ag2O/Ag2CO3/MWNTs Composite Photocatalysts for Enhancement of Ciprofloxacin Degradation, Applied surface science, 366: 1-8 (2016).
[24] Lai C., Zhang M., Li B., Huang D., Zeng G., Qin L., Liu X., Yi H., Cheng M., Li L., Chen Z., Chen L., Fabrication of CuS/BiVO4 (0 4 0) Binary Heterojunction Photocatalysts with Enhanced Photocatalytic Activity for Ciprofloxacin Degradation and Mechanism Insight, Chemical Engineering Journal, 358: 891-902 (2019).
[25] Kyzas G.Z., Koltsakidou A., Nanaki S.G., Bikiaris D.N., Lambropoulou D.A., Removal of Beta-Blockers from Aqueous Media by Adsorption onto Graphene Oxide, Science of The Total Environment, 537: 411-420 (2015).
[26] Abdel Maksoud M.I.A., Fahim R.A., Bedir A.G., Osman A.I., Abouelela M.M., El-Sayyad G.S., Elkodous M.A., Mahmoud A.S., Rabee M.M., Al-Muhtaseb A.a.H., Rooney D.W., Engineered Magnetic Oxides Nanoparticles as Efficient Sorbents for Wastewater Remediation: A Review, Environmental Chemistry Letters, 20(1): 519-562 (2022).
[27] Jiang M., Yang W., Zhang Z., Yang Z., Wang Y., Adsorption of Three Pharmaceuticals on two Magnetic Ion-Exchange Resins, Journal of Environmental Sciences, 31: 226-234 (2015).
[28] Rakić V., Rajić N., Daković A., Auroux A., The Adsorption of Salicylic Acid, Acetylsalicylic Acid and Atenolol from Aqueous Solutions onto Natural Zeolites and Clays: Clinoptilolite, Bentonite and Kaolin, Microporous and Mesoporous Materials, 166: 185-194 (2013).
[32] Wang S., Sun H., Ang H.M., Tadé M.O., Adsorptive Remediation of Environmental Pollutants Using Novel Graphene-Based Nanomaterials, Chemical Engineering Journal, 226: 336-347 (2013).
[33] Al-Khateeb L.A., Almotiry S., Salam M.A., Adsorption of Pharmaceutical Pollutants onto Graphene Nanoplatelets, Chemical Engineering Journal, 248: 191-199 (2014).
[35] Park S., An J., Potts J.R., Velamakanni A., Murali S., Ruoff R.S., Hydrazine-Reduction of Graphite- and Graphene Oxide, Carbon, 49(9): 3019-3023 (2011).
[36] Pei S., Cheng H.-M., The Reduction of Graphene Oxide, Carbon, 50(9): 3210-3228 (2012).
[37] Matsumoto Y., Koinuma M., Kim S.Y., Watanabe Y., Taniguchi T., Hatakeyama K., Tateishi H., Ida S., Simple Photoreduction of Graphene Oxide Nanosheet under Mild Conditions, ACS Applied Materials & Interfaces, 2(12): 3461-3466 (2010).
 [39] Ghosh D., Giri S., Moniruzzaman M., Basu T., Mandal M., Das C.K., α MnMoO4/Graphene Hybrid Composite: High Energy Density Supercapacitor Electrode Material, Dalton Transactions, 43(28): 11067-11076 (2014).
[40] Yang Y., Luo L., Xiao M., Li H., Pan X., Jiang F., One-Step Hydrothermal Synthesis of Surface Fluorinated TiO2/Reduced Graphene Oxide Nanocomposites for Photocatalytic Degradation of Estrogens, Materials Science in Semiconductor Processing, 40: 183-193 (2015).
[41] Shen J., Shi M., Yan B., Ma H., Li N., Ye M., One-Pot Hydrothermal Synthesis of Ag-Reduced Graphene Oxide Composite With Ionic Liquid, Journal of Materials Chemistry, 21(21): 7795-7801 (2011).
[42] Dong S., Pi Y., Li Q., Hu L., Li Y., Han X., Wang J., Sun J., Solar Photocatalytic Degradation of Sulfanilamide by BiOCl/Reduced Graphene Oxide Nanocomposites: Mechanism and Degradation Pathways, Journal of Alloys and Compounds, 663: 1-9 (2016).
[43] Yang S., Yue W., Huang D., Chen C., Lin H., Yang X., A Facile Green Strategy for Rapid Reduction of Graphene Oxide by Metallic Zinc, RSC Advances, 2(23): 8827-8832 (2012).
[44] Xiang Q., Yu J., Jaroniec M., Enhanced Photocatalytic H2-Production Activity of Graphene-Modified Titania Nanosheets, Nanoscale, 3(9): 3670-3678 (2011).
[45] Perera S.D., Mariano R.G., Vu K., Nour N., Seitz O., Chabal Y., Balkus K.J., Hydrothermal Synthesis of Graphene-TiO2 Nanotube Composites with Enhanced Photocatalytic Activity, ACS Catalysis, 2(6): 949-956 (2012).
[48] Avcı A., İnci İ., Baylan N., A Comparative Adsorption Study with Various Adsorbents for the Removal of Ciprofloxacin Hydrochloride from Water, Water, Air, & Soil Pollution, 230(10): 250 (2019).
[49] Avcı A., İnci İ., Baylan N., Adsorption of Ciprofloxacin Hydrochloride on Multiwall Carbon Nanotube, Journal of Molecular Structure, 1206: 127711 (2020).
[50] Maheshwari M., Vyas R.K., Sharma M., Kinetics, Equilibrium and Thermodynamics of Ciprofloxacin Hydrochloride Removal by Adsorption on Coal Fly Ash and Activated Alumina, Desalination and Water Treatment, 51(37-39): 7241-7254 (2013).
[51] Ngeno E.C., Shikuku V.O., Orata F., Baraza L.D., Kimosop S.J., Caffeine and Ciprofloxacin Adsorption from Water onto Clinoptilolite: Linear Isotherms, Kinetics, Thermodynamic and Mechanistic Studies, South African Journal of Chemistry, 72: 136-142 (2019).