Synthesis of Chitosan/Graphene Oxide-Ferric Oxide Composite via Coprecipitation: An Upgraded Adsorbent Material for Methylene Blue Dye Removal
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محتوى المقالة الرئيسي
الملخص
This study addresses the critical need for effective dye removal in wastewater treatment by developing a chitosan/graphene oxide-ferric oxide (CS/GO-Fe2O₃) composite through a coprecipitation method. The primary objective was to evaluate its adsorption performance for methylene blue (MB), a model cationic dye, while optimizing key operational parameters. The composite was systematically characterized using X-ray diffraction (XRD), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), and Brunauer-Emmett-Teller (BET) analysis. XRD patterns confirmed the integration of crystalline Fe2O₃ nanoparticles with a crystallite size of 19.25 nm within the composite matrix, while SEM-EDS revealed a transformation from a dense chitosan morphology to a highly porous structure in the CS/GO-Fe2O₃ composite enriched with carbon, oxygen, nitrogen, and iron. BET analysis demonstrated a substantially higher surface area than that of conventional adsorbents, increasing from 7.036 m²/g for pure chitosan to 39.946 m²/g for the composite. Adsorption studies identified the optimal conditions at pH 9 and a contact time of 50 minutes. The composite exhibited superior adsorption capacity relative to many reported materials, following the Langmuir isotherm model, which has a maximum adsorption capacity (Qm) of 11.655 mg/g. These findings highlight the composite’s potential as a cost-effective and magnetically separable adsorbent for environmental remediation, offering insights into the design of hybrid materials for organic pollutant removal.
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THIS IS AN OPEN ACCESS ARTICLE UNDER THE CC BY LICENSE http://creativecommons.org/licenses/by/4.0/
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المراجع
Kusumlata, Ambade B, Kumar A, Gautam S. Sustainable Solutions: Reviewing the Future of Textile Dye Contaminant Removal with Emerging Biological Treatments. Limnological Review 2024; 24: 126-149.
Oladoye PO, Ajiboye TO, Omotola EO, Oyewola OJ. Methylene Blue Dye: Toxicity and Potential Elimination Technology from Wastewater. Results in Engineering 2022; 16: 1-17.
Khan I, Saeed K, Zekker I, Zhang B, Hendi AH, Ahmad A, Ahmad S, Zada N, Ahmad H, Shah LA, Shah T, Khan I. Review on Methylene Blue: Its Properties, Uses, Toxicity and Photodegradation. Water 2022; 14(2): 242.
Zein R, Purnomo SJ, Ramadhani P, Safni, Alif MF, Putri CN. Enhancing Sorption Capacity of Methylene Blue Dye Using Solid Waste of Lemongrass Biosorbent by Modification Method. Arabian Journal of Chemistry 2023; 16(2): 104480.
Kumari H, Sonia, Suman, Ranga R, Chahal S, Devi S, Sharma S, Kumar S, Kumar P, Kumar S, Kumar A, Parmar R. A Review on Photocatalysis Used for Wastewater Treatment: Dye Degradation. Water, Air, & Soil Pollution 2023; 234(6): 349.
Fouda-Mbanga BG, Onotu OP, Tywabi-Ngeva Z. Advantages of the Reuse of Spent Adsorbents and Potential Applications in Environmental Remediation: A Review. Green Analytical Chemistry 2024; 11: 100156.
Despina AG, Athanasia KT, Ioannis AK, George ZK. The Adsorption-Desorption-Regeneration Pathway to a Circular Economy: The Role of Waste-Derived Adsorbents on Chromium Removal. Separation and Purification Technology 2025; 368: 132996.
Graça NS, Rodrigues AE. The Combined Implementation of Electrocoagulation and Adsorption Processes for the Treatment of Wastewaters. Clean Technologies 2022; 4: 1020-1053.
Garcia RV, Silva ML, Oliveira VEM, Martins VCC, Araújo JF, Prata EG, Correia LM. Materials for Methylene Blue Adsorption. Research, Society and Development 2021; 10(9): e37410918114.
Wang L, Yuan Z, Wen F, Cheng Y, Zhang Y, Wang G. A Bipolar Passive DMFC Stack for Portable Applications. Energy 2018; 144: 587–593.
Jiménez-Gómez CP, Cecilia JA. Chitosan: A Natural Biopolymer with a Wide and Varied Range of Applications. Molecules 2020; 25(17): 3981.
Nikoshvili LZ, Tikhonov BB, Ivanov PE, Stadolnikova PY, Sulman MG, Matveeva VG. Recent Progress in Chitosan-Containing Composite Materials for Sustainable Approaches to Adsorption and Catalysis. Catalysts 2023; 13: 367.
Dan S, Bagheri H, Shahidizadeh A, Hashemipour H. Performance of Graphene Oxide/SiO2 Nanocomposite-based: Antibacterial Activity, Dye and Heavy Metal Removal. Arabian Journal of Chemistry 2023; 16(2): 104450.
Jayaramulu K, Mukherjee S, Morales DM, Dubal DP, Nanjundan AK, Schneemann A, Masa J, Kment S, Schuhmann W, Otyepka M, Zbořil R, Fischer RA. Graphene-Based Metal–Organic Framework Hybrids for Applications in Catalysis, Environmental, and Energy Technologies. Chemical Reviews 2022; 122(24): 17241-17338.
Luong HVT, Le TP, Le TLT, Dang HG, Tran TBQ. A Graphene Oxide Based Composite Granule for Methylene Blue Separation from Aqueous Solution: Adsorption, Kinetics and Thermodynamic Studies. Heliyon 2024; 10(7): e28648.
Aswini R, Hartati S, Jothimani K, Pothu R, Shanmugam P, Lee Y, Masimukku S, Boddula R, Selvaraj M, Al-Qahtani N. Revolutionizing Microorganism Inactivation: Magnetic Nanomaterials in Sustainable Photocatalytic Disinfection. Journal of Environmental Management 2024; 370: 122738.
Shan H, Zeng C, Zhao C, Zhan H. Iron Oxides Decorated Graphene Oxide/chitosan Composite Beads for Enhanced Cr(VI) Removal from Aqueous Solution. International Journal of Biological Macromolecules 2021; 172: 197-209.
Zhong X, Lv N, Zhang M, Tan Y, Yuan Q, Hu C, Ma M, Wu Y, Ouyang J. Magnetic β-Cyclodextrin Polymer Nanoparticles for Efficient Adsorption of U(VI) from Wastewater. Crystals 2023; 13: 1496.
Joseph J, Iftekhar S, Srivastava V, Fallah Z, Zare EN, Sillanpää M. Iron-based Metal-organic Framework: Synthesis, Structure and Current Technologies for Water Reclamation with Deep Insight into Framework Integrity. Chemosphere 2021; 284: 131171.
Pourmadadi M, Rahmani E, Shamsabadipour A, Mahtabian S, Ahmadi M, Rahdar A, Díez-Pascual AM. Role of Iron Oxide Nanocomposites in Advanced Biomedical Applications: A State-of-the-Art Review. Nanomaterials 2022; 12(21): 3873.
Nayl AA, Abd-Elhamid AI, Arafa WAA, Ahmed IM, El-Shanshory AA, Abu-Saied MA, Soliman HMA, Abdelgawad MA, Ali HM, Bräse S. Chitosan-Functionalized-Graphene Oxide (GO@CS) Beads as an Effective Adsorbent to Remove Cationic Dye from Wastewater. Polymers 2022; 14(19): 4236.
Hernandez JST, Aragón-Muriel A, Corrales Quintero W, Castro Velásquez JC, Salazar-Camacho NA, Pérez Alcázar GA, Tabares JA. Characterization of Fe3O4 Nanoparticles for Applications in Catalytic Activity in the Adsorption/Degradation of Methylene Blue and Esterification. Molecules 2022; 27(24): 8976.
Meng X, Xu Y, Sun X, Xiong L, Wang Q. Nitrogen-doped Graphene Assists Fe2O3 in Enhancing Electrochemical Performance. Journal of Power Sources 2016; 326: 389–396.
Bulin C, Li B, Zhang Y, Zhang B. Removal Performance and Mechanism of Nano α-Fe2O3/graphene Oxide on Aqueous Cr(VI). Journal of Physics and Chemistry of Solids 2020; 147: 109659.
Le D, Carbonnier B, Hamadi S, Grande D, Fois M, Naili S, Nguyen V, Mahouche-Chergui S. Toward the Development of Graphene/Chitosan Biocomposite Aerogels with Enhanced Mechanical and Thermal Insulation Performance. ACS Applied Polymer Materials 2024; 6(21): 13132-13146.
Hussain S, Maktedar SS. Structural, Functional and Mechanical Performance of Advanced Graphene-based Composite Hydrogels. Results in Chemistry 2023; 6: 101029.
Ullah T, Gul K, Khan H, Ara B, Zia TUH. Efficient Removal of Selected Fluoroquinolones from the Aqueous Environment Using Reduced Magnetic Graphene Oxide/Polyaniline Composite. Chemosphere 2022; 293: 133452.
Liu X, Zhao X, Liu Y, Zhang T. Review on Preparation and Adsorption Properties of Chitosan and Chitosan Composites. Polymer Bulletin 2022; 79(4): 2633–2665.
Liu Y, Shan H, Zeng C, Zhan H, Pang Y. Removal of Cr(VI) from Wastewater Using Graphene Oxide Chitosan Microspheres Modified with α–FeO(OH). Materials 2022; 15(14): 4949.
Saputra AMA, Agustina N, Amran, Zurnansyah, Samnur, Sujiono EH. Synthesis and Characterisation of Graphene Oxide/Chitosan Composite Membranes from Natural Waste. Journal of Physical Science 2022; 33(3): 63–79.
Dhull P, Lohchab RK, Kumari M, Singh K, Bhankhar AK, Shaloo. A Facile Method for Synthesis of α-Fe2O3 Nanoparticles and Assessment of Their Characterization. Nature Environment and Pollution Technology 2024; 23(1): 321-330.
Mpelane S, Mketo N, Mlambo M, Bingwa N, Nomngongo PN. One-Step Synthesis of a Mn-Doped Fe2O3/GO Core-Shell Nanocomposite and Its Application for the Adsorption of Levofloxacin in Aqueous Solution. ACS Omega 2022; 7(27): 23302-23314.
Vanitha C, Sucharitha M, Anandhavelu S, Sethuraman V, Yogananth A. One-pot Synthesis of Chitosan@cofe2o3-graphene Oxidenanocomposites as Electrode Materials for Electrochemical Biosensor and Super Capacitor. Digest Journal of Nanomaterials and Biostructures 2021; 16(1): 151-160.
Modau L, Sigwadi R, Mokrani T, Nemavhola F. Chitosan Membranes for Direct Methanol Fuel Cell Applications. Membranes 2023; 13(10): 838.
Abou EA, Ibrahim AMM, El Sayed AM. Influence of α-Fe2O3, CuO and GO 2D Nano-fillers on the Structure, Physical Properties and Antifungal Activity of Na-CMC–PAAm Blend. Scientific Reports 2023; 13: 12358.
Zhu W, Jiang X, Liu F, You F, Yao C. Preparation of Chitosan-Graphene Oxide Composite Aerogel by Hydrothermal Method and Its Adsorption Property of Methyl Orange. Polymers 2020; 12(9): 2169.
Sabzevari M, Cree DE, Wilson LD. Graphene Oxide-Chitosan Composite Material for Treatment of a Model Dye Effluent. ACS Omega 2018; 3(10): 13045-13054.
Liu W, Zhang Y, Wang S, Bai L, Deng Y, Tao J. Effect of Pore Size Distribution and Amination on Adsorption Capacities of Polymeric Adsorbents. Molecules 2021; 26(17): 5267.
Hoang VT, Lieu TB, Thuy TD, Dang HL, Chinh DH, Anh XT. Graphene Oxide/Fe3O4/chitosan Nanocomposite: A Recoverable and Recyclable Adsorbent for Organic Dyes Removal. Application to Methylene Blue. Materials Research Express 2017; 4: 035701.
Huimei S, Chunya Z, Chaoran Z, Hongbin Z. Iron Oxides Decorated Graphene Oxide/Chitosan Composite Beads for Enhanced Cr(VI) Removal from Aqueous Solution. International Journal of Biological Macromolecules 2021; 172: 197–209.
Hanafi MF, Sapawe N. Effect of pH on the Photocatalytic Degradation of Remazol Brilliant Blue Dye Using Zirconia Catalyst. Materials Today: Proceedings 2020; 31: 260–262.
Wahyuni S, Nasrudin N, Muhamad BJ, Permana D. Fabrication of Chitosan/Fe3O4 Nanocomposite as Adsorbent for Reduction Methylene Blue Contents. Indonesian Journal of Chemistry 2022; 22(3): 878-886.
Broujeni R, Nilchi A, Hassani A, Saberi R. Preparation and Characterization of Chitosan/Fe3O4 Nanocomposites for the Adsorption of Thorium (IV) Ion from Aqueous Solution. Water Science and Technology 2018; 78(3): 708-720.
Sumanjit, Rani S, Mahajan RK. Equilibrium, Kinetics and Thermodynamic Parameters for Adsorptive Removal of Dye Basic Blue 9 by Ground Nut Shells and Eichhornia. Arabian Journal of Chemistry 2016; 9: S1464-S1477.
Baunsele AB, Boelan EG, Kopon AM, Rahayu, Siswanta D. Kinetic Study of Blue Methylene Adsorption Using Coconut Husk Base Activated. Indonesian Journal of Chemical Research 2022; 10(2): 111-117.
Zhang B, Hu R, Sun D. Fabrication of Chitosan/magnetite-graphene Oxide Composites as a Novel Bioadsorbent for Adsorption and Detoxification of Cr(VI) from Aqueous Solution. Scientific Reports 2018; 8: 15397.
Ramadhani ED, Kurniawati D. Effect of Contact Time and Agitation Speed on the Adsorption Process of Methylene Blue Dyes Using Longan Shell (Euphoria longan L.) as Biosorbent. American Journal of Sciences and Engineering Research 2021; 4(6): 143-149.
Dinh HT, Tran NT, Trinh DX. Investigation into the Adsorption of Methylene Blue and Methyl Orange by UiO-66 Nanoparticles. Journal of Analytical Methods in Chemistry 2021; 2021: 5512174.
Bazrafshan E, Mostafapour FK, Zazouli MA. Methylene Blue (Cationic Dye) Adsorption into Salvadora persica Stems Ash. African Journal of Biotechnology 2012; 11(101): 16661–16668.
Alharby NF, Almutairi RS, Mohamed NA. Adsorption Behavior of Methylene Blue Dye by Novel CrossLinked O-CM-Chitosan Hydrogel in Aqueous Solution: Kinetics, Isotherm and Thermodynamics. Polymers 2021; 13(21): 3659.
Kalam S, Abu-Khamsin SA, Kamal MS, Patil S. Surfactant Adsorption Isotherms: A Review. ACS Omega 2021; 6(48): 32342-32348.
Murphy OP, Vashishtha M, Palanisamy P, Kumar KV. A Review on the Adsorption Isotherms and Design Calculations for the Optimization of Adsorbent Mass and Contact Time. ACS Omega 2023; 8(20): 17407-17430.
Gawande SM, Belwalkar NS, Mane AA. Adsorption and its Isotherm – Theory. International Journal of Engineering Research 2017; 6(6): 312.
Side S, Perdana R, Putri SE, Pratiwi DE. Methylene Blue Adsorption Study Using Zeolite-PBO Composite. Journal of Applied Chemical Science International 2023; 16(2): 24–31.
Afzal H, Masood MH, Ali N. Advancing Environmental Sustainability: Optimizing the Application of Activated Carbon from Sugarcane Trash and Cotton Seed Waste for Methylene Blue Adsorption. Tikrit Journal of Engineering Sciences 2025; 32(4): 1907.
Baunsele AB, Miss H. Langmuir and Freundlich Equation Test on Methylene Blue Adsorption by Using Coconut Fiber Biosorbent. Walisongo Journal of Chemistry 2021; 4(2): 131–138.
Kalaiselvi D, Sangeetha V, Basker A, Saravanan D, Kandavelu V. Biotreatment of a Triphenylmethane Dye Solution Using Medicinal Plant Rhizome: Acorus calamus. Research Journal of Chemical Sciences 2015; 5(4): 13–19.