Skip to main content
SpringerLink
Log in

Process Optimization and Adsorptive Mechanism for Reactive Blue 19 Dye by Magnetic Crosslinked Chitosan/MgO/Fe3O4 Biocomposite

  • Original Paper
  • Published:
Journal of Polymers and the Environment Aims and scope Submit manuscript

Abstract

A new biocomposite cross-linked glutaraldehyde-chitosan/MgO/Fe3O4 (CTS-GL/MgO/Fe3O4) adsorbent with magneto-responsiveness was prepared and applied for the removal of reactive blue 19 (RB-19), a synthetic textile dye. The prepared CTS-GL/MgO/Fe3O4 was structurally characterized using spectroscopic (XRD, FTIR, SEM–EDX), and its physicochemical properties were evaluated using potentiometry and pHpzc analyses. The influence of various adsorption parameters (A: CTS-GL/MgO/Fe3O4 dosage; B: initial solution pH; C: process temperature; and D: contact time) on the removal efficiency of RB-19 was statistically optimized using Box-Behnken design (BBD). The analysis of variance (ANOVA) indicates the presence of five significant statistical interactions between the adsorption parameters, as follows: AB, AC, AD, BC, and BD. The equilibrium dye uptake by the Freundlich isotherm model indicates heterogeneous adsorption, while the kinetics of adsorption was well-described by the pseudo-second-order model. The maximum adsorption capacity of CTS-GL/MgO/Fe3O4 towards RB-19 was 193.2 mg/g at 45 °C. This work highlights the development of a recoverable magnetic biocomposite adsorbent with favourable adsorption capacity towards a model textile dye with good separation ability by using an external magnetic field. Moreover, separation of the magnetic adsorbents from the treated solution is easy and convenient apply to continuous flow systems, which is highly preferred for industrial applications.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

Data Availability

The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

References

  1. Jawad AH, Abdulhameed AS, Wilson LD, Hanafah MAKM, Nawawi WI, ALOthman ZA, Khan MR (2021) J Polym Environ 29:2855–2868

    Article  CAS  Google Scholar 

  2. Tkaczyk A, Mitrowska K, Posyniak A (2020) Synthetic organic dyes as contaminants of the aquatic environment and their implications for ecosystems: a review. Sci Total Environ 717:137222

    Article  CAS  PubMed  Google Scholar 

  3. Rafaie HA, Yusop NFM, Azmi NF, Abdullah NS, Ramli NIT (2021) Photocatalytic degradation of methylene blue dye solution using different amount of ZnO as a photocatalyst. Sci Lett 15(1):1–12

    Article  Google Scholar 

  4. Rashid RA, Ishak MAM, Mohammed K (2018) Adsorptive removal of methylene blue by commercial coconut shell activated carbon. Sci Lett 12(1):77–101

    Google Scholar 

  5. Malek NNA, Mohammed IA, Reghioua A, Yousif E, Jawad AH (2020) Removal of reactive red 4 dye using chitosan- epichlorohydrin/ TiO2 nanocomposite: application of response surface methodology. Sci Lett 14(1):96–108

    Google Scholar 

  6. Benkhaya S, M’rabet S, El Harfi A (2020) Classifications, properties, recent synthesis and applications of azo dyes. Heliyon 6(1):03271

    Article  Google Scholar 

  7. Li Y, Li Z, Xia Y, Li H, Shi J, Zhang A, Gao L (2020) Fabrication of ternary AgBr/BiPO4/g-C3N4 heterostructure with dual Z-scheme and its visible light photocatalytic activity for Reactive Blue 19. Environ Res 192:110260

    Article  PubMed  CAS  Google Scholar 

  8. Ao C, Zhao J, Li Q, Zhang J, Huang B, Wang Q, Lu C (2020) Biodegradable all-cellulose composite membranes for simultaneous oil/water separation and dye removal from water. Carbohydr Polym 250:116872

    Article  CAS  PubMed  Google Scholar 

  9. Cojocaru C, Clima L (2020) Polymer assisted ultrafiltration of AO7 anionic dye from aqueous solutions: experimental design, multivariate optimization, and molecular docking insights. J Membr Sci 604:118054

    Article  CAS  Google Scholar 

  10. Feng Q, Gao B, Yue Q, Guo K (2020) Flocculation performance of papermaking sludge-based flocculants in different dye wastewater treatment: comparison with commercial lignin and coagulants. Chemosphere 262:128416

    Article  PubMed  CAS  Google Scholar 

  11. Varjani S, Rakholiya P, Ng HY, You S, Teixeira JA (2020) Microbial degradation of dyes: an overview. Bioresour Technol 314:123728

    Article  CAS  PubMed  Google Scholar 

  12. Ghaffari Y, Gupta NK, Bae J, Kim KS (2020) One-step fabrication of Fe2O3/Mn2O3 nanocomposite for rapid photodegradation of organic dyes at neutral pH. J Mol Liq 315:113691

    Article  CAS  Google Scholar 

  13. Jawad AH, Abdulhameed AS, Reghioua A, Yaseen ZM (2020) Zwitterion composite chitosan-epichlorohydrin/zeolite for adsorption of methylene blue and reactive red 120 dyes. Int J Biol Macromol 163:756–765

    Article  CAS  PubMed  Google Scholar 

  14. Surip SN, Abdulhameed AS, Garba ZN, Syed-Hassan SSA, Ismail K, Jawad AH (2020) H2SO4-treated Malaysian low rank coal for methylene blue dye decolourization and cod reduction: Optimization of adsorption and mechanism study. Surf Interface 21:100641

    Article  CAS  Google Scholar 

  15. Upadhyay U, Sreedhar I, Singh SA, Patel CM, Anitha KL (2020) Recent advances in heavy metal removal by chitosan based adsorbents. Carbohydr Polym 251:117000

    Article  PubMed  CAS  Google Scholar 

  16. Liu C, Bai R (2014) Recent advances in chitosan and its derivatives as adsorbents for removal of pollutants from water and wastewater. Curr Opin Chem Eng 4:62–70

    Article  Google Scholar 

  17. Jawad AH, Abdulhameed AS, Malek NNA, ALOthman ZA (2020) Statistical optimization and modeling for color removal and COD reduction of reactive blue 19 dye by mesoporous chitosan-epichlorohydrin/kaolin clay composite. Int J Biol Macromol 164:4218–4230

    Article  CAS  PubMed  Google Scholar 

  18. Saheed IO, Da OW, Suah FBM (2021) Chitosan modifications for adsorption of pollutants-a review. J Hazard Mater. 408:124889

    Article  CAS  PubMed  Google Scholar 

  19. Gul K, Sohni S, Waqar M, Ahmad F, Norulaini NN, Ak MO (2016) Functionalization of magnetic chitosan with graphene oxide for removal of cationic and anionic dyes from aqueous solution. Carbohydr Polym 152:520–531

    Article  CAS  PubMed  Google Scholar 

  20. Jawad AH, Mubarak NSA, Abdulhameed AS (2020) Tunable Schiff’s base-cross-linked chitosan composite for the removal of reactive red 120 dye: adsorption and mechanism study. Int J Biol Macromol 142:732–741

    Article  CAS  PubMed  Google Scholar 

  21. Vakili M, Mojiri A, Zwain HM, Yuan J, Giwa AS, Wang W, Yu G (2019) Effect of beading parameters on cross-linked chitosan adsorptive properties. React Funct Polym 144:104354

    Article  CAS  Google Scholar 

  22. Jawad AH, Mubarak NSA, Abdulhameed AS (2020) Hybrid crosslinked chitosan-epichlorohydrin/TiO2 nanocomposite for reactive red 120 dye adsorption: kinetic, isotherm, thermodynamic, and mechanism study. J Polym Environ 28:624–637

    Article  CAS  Google Scholar 

  23. Nouh SA, Alsobhi BO, Abou Elfadl A, Benthami K, Khalil KD, Riyadh SM (2020) Structure and thermal investigation of the effect of laser radiation in Chitosan-MgO nanocomposite film. Radiat Eff Defects Solids 175(5–6):422–432

    Article  CAS  Google Scholar 

  24. Nga NK, Chau NTT, Viet PH (2020) Preparation and characterization of a chitosan/MgO composite for the effective removal of reactive blue 19 dye from aqueous solution. J Sci 201–202:68–93

    Google Scholar 

  25. Haldorai Y, Shim JJ (2014) An efficient removal of methyl orange dye from aqueous solution by adsorption onto chitosan/MgO composite: a novel reusable adsorbent. Appl Surf Sci 292:447–453

    Article  CAS  Google Scholar 

  26. Wang Y, Cen C, Chen J, Fu L (2020) MgO/carboxymethyl chitosan nanocomposite improves thermal stability, waterproof and antibacterial performance for food packaging. Carbohydra Polym 236:116078

    Article  CAS  Google Scholar 

  27. Huang YZ, Ji YR, Kang ZW, Li F, Ge SF, Yang DP, Fan XQ (2020) Integrating eggshell-derived CaCO3/MgO nanocomposites and chitosan into a biomimetic scaffold for bone regeneration. Chem Eng J 395:125098

    Article  CAS  Google Scholar 

  28. Sundaram CS, Viswanathan N, Meenakshi S (2009) Defluoridation of water using magnesia/chitosan composite. J Hazard Mater 163(2–3):618–624

    Article  PubMed  CAS  Google Scholar 

  29. Patel MK, Ali MA, Zafaryab M, Agrawal VV, Rizvi MMA, Ansari ZA, Malhotra BD (2013) Biocompatible nanostructured magnesium oxide-chitosan platform for genosensing application. Biosens Bioelectron 45:181–188

    Article  CAS  PubMed  Google Scholar 

  30. Riyadh SM, Khalil KD, Aljuhani A (2018) Chitosan-MgO nanocomposite: one pot preparation and its utility as an ecofriendly biocatalyst in the synthesis of thiazoles and [1, 3, 4] thiadiazoles. Nanomaterials 8(11):928

    Article  PubMed Central  CAS  Google Scholar 

  31. Reddy DHK, Lee SM (2013) Application of magnetic chitosan composites for the removal of toxic metal and dyes from aqueous solutions. Adv Colloid Interface Sci 201:68–93

    Article  PubMed  CAS  Google Scholar 

  32. Dalvand A, Nabizadeh R, Ganjali MR, Khoobi M, Nazmara S, Mahvi AH (2016) Modeling of Reactive Blue 19 azo dye removal from colored textile wastewater using L-arginine-functionalized Fe3O4 nanoparticles: optimization, reusability, kinetic and equilibrium studies. J Magn Magn Mater 404:179–189

    Article  CAS  Google Scholar 

  33. Vieira RS, Beppu MM (2006) Interaction of natural and crosslinked chitosan membranes with Hg (II) ions. Colloids Surf A 279(1–3):196–207

    Article  CAS  Google Scholar 

  34. Hu YY, Pan C, Zheng X, Hu F, Xu L, Xu G, Peng X (2020) Prediction and optimization of adsorption properties for Cs+ on NiSiO@ NiAlFe LDHs hollow spheres from aqueous solution: kinetics, isotherms, and BBD model. J Hazard Mater 401:123374

    Article  PubMed  CAS  Google Scholar 

  35. Sing KS (1985) Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984). Pure Appl Chem 57(4):603–619

    Article  CAS  Google Scholar 

  36. Chen L, Wu P, Chen M, Lai X, Ahmed Z, Zhu N, Liu T (2018) Preparation and characterization of the eco-friendly chitosan/vermiculite biocomposite with excellent removal capacity for cadmium and lead. Appl Clay Sci 159:74–82

    Article  CAS  Google Scholar 

  37. dos Santos JM, Pereira CR, Pinto LAA, Frantz T, Lima ÉC, Foletto EL, Dotto GL (2019) Synthesis of a novel CoFe2O4/chitosan magnetic composite for fast adsorption of indigotine blue dye. Carbohydr Polym 217:6–14

    Article  PubMed  CAS  Google Scholar 

  38. Yang Y, Ali N, Khan A, Khan S, Khan S, Khan H, Bilal M (2020) Chitosan-capped ternary metal selenide nanocatalysts for efficient degradation of carcinogenic Congo red dye in sunlight irradiation. Int J Biol Macromol 167:169–181

    Article  PubMed  CAS  Google Scholar 

  39. Jaafari J, Barzanouni H, Mazloomi S, Farahani NAA, Sharafi K, Soleimani P, Haghighat GA (2020) Effective adsorptive removal of reactive dyes by magnetic chitosan nanoparticles: kinetic, isothermal studies and response surface methodology. Int J Boil Macromol 164:344–355

    Article  CAS  Google Scholar 

  40. Naeeji N, Shahbazi Y, Shavisi N (2020) Effect of gamma irradiation on physico-mechanical and structural properties of basil seed mucilage-chitosan films containing Ziziphora clinopodioides essential oil and MgO nanoparticles for rainbow trout packaging. J Food Process Preserv 44(10):14781

    Article  CAS  Google Scholar 

  41. Pereira MBB, França DB, Araújo RC, Silva Filho EC, Rigaud B, Fonseca MG, Jaber M (2020) Amino hydroxyapatite/chitosan hybrids reticulated with glutaraldehyde at different pH values and their use for diclofenac removal. Carbohyd Polym 236:116036

    Article  CAS  Google Scholar 

  42. Jawad AH, Abdulhameed AS (2020) Facile synthesis of crosslinked chitosan-tripolyphosphate/kaolin clay composite for decolourization and COD reduction of remazol brilliant blue R dye: optimization by using response surface methodology. Colloids Surf A 605:125329

    Article  CAS  Google Scholar 

  43. Jawad AH, Abdulhameed AS (2020) Statistical modeling of methylene blue dye adsorption by high surface area mesoporous activated carbon from bamboo chip using KOH-assisted thermal activation. Energy Ecol Environ 5(6):456–469

    Article  Google Scholar 

  44. Abdulhameed AS, Mohammad AT, Jawad AH (2019) Application of response surface methodology for enhanced synthesis of chitosan tripolyphosphate/TiO2 nanocomposite and adsorption of reactive orange 16 dye. J Clean Prod 232:43–56

    Article  CAS  Google Scholar 

  45. Jawad AH, Malek NNA, Abdulhameed AS, Razuan R (2020) Synthesis of magnetic chitosan-fly Ash/Fe3O4 composite for adsorption of reactive orange 16 Dye: optimization by Box-Behnken design. J Polym Environ 28(3):1068–1082

    Article  CAS  Google Scholar 

  46. Kausar A, Sher F, Hazafa A, Javed A, Sillanpää M, Iqbal M (2020) Biocomposite of sodium-alginate with acidified clay for wastewater treatment: kinetic, equilibrium and thermodynamic studies. Int J Biol Macromol 161:1272–1285

    Article  CAS  PubMed  Google Scholar 

  47. Kalhori EM, Al-Musawi TJ, Ghahramani E, Kazemian H, Zarrabi M (2017) Enhancement of the adsorption capacity of the light-weight expanded clay aggregate surface for the metronidazole antibiotic by coating with MgO nanoparticles: studies on the kinetic, isotherm, and effects of environmental parameters. Chemosphere 175:8–20

    Article  CAS  PubMed  Google Scholar 

  48. Njoku VO, Islam MA, Asif M, Hameed BH (2014) Preparation of mesoporous activated carbon from coconut frond for the adsorption of carbofuran insecticide. J Anal Appl Pyrol 110:172–180

    Article  CAS  Google Scholar 

  49. Lagergren S (1898) Zur theorie der sogenannten adsorption geloster stoffe. Vet Akad Handl 24:1–39

    Google Scholar 

  50. Ho YS, McKay G (1998) Sorption of dye from aqueous solution by peat. Chem Eng J 70:115–124

    Article  CAS  Google Scholar 

  51. Huang L, Yang Z, Lei D, Liu F, He Y, Wang H, Luo J (2020) Experimental and modeling studies for adsorbing different species of fluoride using lanthanum-aluminum perovskite. Chemosphere 263:128089

    Article  PubMed  CAS  Google Scholar 

  52. Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403

    Article  CAS  Google Scholar 

  53. Freundlich HMF (1906) Over the adsorption in solution. J Phys Chem 57:385–471

    CAS  Google Scholar 

  54. Temkin MI (1940) Kinetics of ammonia synthesis on promoted iron catalysts. Acta Physiochim URSS 12:327–356

    CAS  Google Scholar 

  55. Chen J, Hu H, Yang J, Xue H, Tian Y, Fan K, Liu Y (2020) Removal behaviors and mechanisms for series of azo dye wastewater by novel nano constructed macro-architectures material. Bioresour Technol 322:124556

    Article  PubMed  CAS  Google Scholar 

  56. Vijayaraghavan K, Won SW, Yun YS (2009) Treatment of complex Remazol dye effluent using sawdust-and coal-based activated carbons. J Hazard Mater 167(1–3):790–796

    Article  CAS  PubMed  Google Scholar 

  57. Janaki V, Oh BT, Shanthi K, Lee KJ, Ramasamy AK, Kamala-Kannan S (2012) Polyaniline/chitosan composite: an eco-friendly polymer for enhanced removal of dyes from aqueous solution. Synth Met 162(11–12):974–980

    Article  CAS  Google Scholar 

  58. Phan DN, Rebia RA, Saito Y, Kharaghani D, Khatri M, Tanaka T, Kim IS (2020) Zinc oxide nanoparticles attached to polyacrylonitrile nanofibers with hinokitiol as gluing agent for synergistic antibacterial activities and effective dye removal. J Ind Eng Chem 85:258–268

    Article  CAS  Google Scholar 

  59. Nair V, Panigrahy A, Vinu R (2014) Development of novel chitosan–lignin composites for adsorption of dyes and metal ions from wastewater. Chem Eng J 254:491–502

    Article  CAS  Google Scholar 

  60. Abbasi M (2017) Synthesis and characterization of magnetic nanocomposite of chitosan/ SiO2/carbon nanotubes and its application for dyes removal. J Clean Prod 145:105–113

    Article  CAS  Google Scholar 

  61. Chinoune K, Bentaleb K, Bouberka Z, Nadim A, Maschke U (2016) Adsorption of reactive dyes from aqueous solution by dirty bentonite. Appl Clay Sci 123:64–75

    Article  CAS  Google Scholar 

  62. Silva MM, Oliveira MM, Avelino MC, Fonseca MG, Almeida RK, Silva Filho EC (2012) Adsorption of an industrial anionic dye by modified-KSF-montmorillonite: evaluation of the kinetic, thermodynamic and equilibrium data. Chem Eng J 203:259–268

    Article  CAS  Google Scholar 

  63. Mate CJ, Mishra S (2020) Synthesis of borax cross-linked Jhingan gum hydrogel for remediation of Remazol Brilliant Blue R (RBBR) dye from water: adsorption isotherm, kinetic, thermodynamic and biodegradation studies. Int J Biol Macromol 151:677–690

    Article  CAS  PubMed  Google Scholar 

Download references

Acknowledgements

The authors are thankful to the Ministry of Higher Education (MOHE), Malaysia, for funding this project under Fundamental Research Grant Scheme (FRGS) no. (Ref: FRGS/1/2019/STG01/UITM/02/3). The authors would like to thank the Faculty of Applied Sciences, Universiti Teknologi MARA, Shah Alam for all facilities. The authors would like to thank Mrs. Nurfarah Farini Binti Muhamad Kamarazzaman, Penolong Pegawai Sains (Assistant Science Officer) at Applied Sciences, Universiti Teknologi MARA, Shah Alam for facilitating XRD analysis. Zeid A. ALOthman is grateful to the Researchers Supporting Project No. (RSP-2021/1), King Saud University, Riyadh, Saudi Arabia.

Funding

This work was supported by Ministry of Higher Education (MOHE) under Fundamental Research Grant Scheme (FRGS) no. (Ref: FRGS/1/2019/STG01/ UITM/02/3), and Researchers Supporting Project No. (RSP-2021/1), King Saud University, Riyadh Saudi Arabia.

Author information

Authors and Affiliations

  1. Faculty of Applied Sciences, Universiti Teknologi MARA, 40450, Shah Alam, Selangor, Malaysia

    Ali H. Jawad

  2. Department of Biotechnology, School of Chemical and Biotechnology, SASTRA Deemed University, Thanjavur, Tamilnadu, 613401, India

    S. Rangabhashiyam

  3. Department of Medical Instrumentation Engineering, Al-Mansour University College, Baghdad, Iraq

    Ahmed Saud Abdulhameed

  4. School of Chemical Engineering, College of Engineering, Universiti Teknologi MARA, 40450, Shah Alam, Selangor, Malaysia

    Syed Shatir A. Syed-Hassan

  5. Chemistry Department, College of Science, King Saud University, Riyadh, 11451, Saudi Arabia

    Zeid A. ALOthman

  6. Department of Chemistry, University of Saskatchewan, Saskatoon, SK, S7N 5C9, Canada

    Lee D. Wilson

Authors
  1. Ali H. Jawad
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. S. Rangabhashiyam
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Ahmed Saud Abdulhameed
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Syed Shatir A. Syed-Hassan
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Zeid A. ALOthman
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Lee D. Wilson
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by AHJ, RS, ASA, SSAS-H, ZAA, LDW. The first draft of the manuscript was written by AHJ, RS, ASA and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Ali H. Jawad.

Ethics declarations

Competing interests

The authors have no relevant financial or non-financial interests to disclose.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jawad, A.H., Rangabhashiyam, S., Abdulhameed, A.S. et al. Process Optimization and Adsorptive Mechanism for Reactive Blue 19 Dye by Magnetic Crosslinked Chitosan/MgO/Fe3O4 Biocomposite. J Polym Environ 30, 2759–2773 (2022). https://doi.org/10.1007/s10924-022-02382-9

Download citation

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10924-022-02382-9

Keywords

Search

Navigation