Skip to main content
SpringerLink
Log in

Magnetic Chitosan-Glutaraldehyde/Zinc Oxide/Fe3O4 Nanocomposite: Optimization and Adsorptive Mechanism of Remazol Brilliant Blue R Dye Removal

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

Abstract

A magnetic Schiff’s base chitosan-glutaraldehyde/Fe3O4 composite (CHT-GLA/ZnO/Fe3O4) was developed by incorporating zinc oxide (ZnO) nanoparticles into its structure to prepare an efficient adsorbent for the removal of remazol brilliant blue R (RBBR) dye. The CHT-GLA/ZnO/Fe3O4 was characterized by the following methods: CHN, BET, FTIR, XRD, SEM–EDX, pHpzc, and potentiometric titrations. Box-Behnken design based on response surface methodology was used to optimize the effects of the A: ZnO nanoparticles loading (0–50%), B: dose (0.02–0.1 g), C: pH (4–10), D: temperature (30–60 °C), and time E: (10–60 min) on the synthesis of the magnetic adsorbent and the RBBR dye adsorption. The experimental data of kinetics followed the pseudo-second order model, while isotherms showed better fit to Freundlich and Temkin models. The maximum adsorption capacity of the target nanocomposite (CHT-GLA/Fe3O4 containing 25% ZnO or CHT-GLA/ZnO/Fe3O4-25) was reached of 176.6 mg/g at 60 °C. The adsorption mechanism of RBBR onto CHT-GLA/ZnO/Fe3O4 nanocomposite can be attributed to multi-interactions including electrostatic attractions, hydrogen bonding, Yoshida H-bonding, and n-π interactions. This study offers a promising hybrid nanobiomaterial adsorbent in environmental nanotechnology to separate and remove the contaminants such as organic dyes from wastewater.

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

References

  1. Pérez-Calderón J, Santos MV, Zaritzky N (2020) Synthesis, characterization and application of cross-linked chitosan/oxalic acid hydrogels to improve azo dye (Reactive Red 195) adsorption. React Funct Polym 155:104699

    Article  CAS  Google Scholar 

  2. 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 

  3. Kueasook R, Rattanachueskul N, Chanlek N, Dechtrirat D, Watcharin W, Amornpitoksuk P, Chuenchom L (2020) Green and facile synthesis of hierarchically porous carbon monoliths via surface self-assembly on sugarcane bagasse scaffold: influence of mesoporosity on efficiency of dye adsorption. Micropor Mesopor Mater 296:110005

    Article  CAS  Google Scholar 

  4. 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 Physicochem Eng Asp 605:125329

    Article  CAS  Google Scholar 

  5. Sathishkumar P, Arulkumar M, Palvannan T (2012) Utilization of agro-industrial waste Jatropha curcas pods as an activated carbon for the adsorption of reactive dye Remazol Brilliant Blue R (RBBR). J Clean Prod 22(1):67–75

    Article  CAS  Google Scholar 

  6. Tang Q, Yang T, Wang S, Cong H-L, Yang X-R, Shen Y-Q, Yu B (2020) Facile light-assisted preparation of reusable magnetic Fe3O4@SiO2@Chitosan composite for adsorption of dyes. Ferroelectrics 562:28–38

    Article  CAS  Google Scholar 

  7. Wang Z, Si Z, Cai D, Li GLS, Qin P (2020) Synthesis of stable COF-300 nanofiltration membrane via in-situ growth with ultrahigh flux for selective dye separation. J Membr Sci 615:118466

    Article  CAS  Google Scholar 

  8. Lakshmanan P, Thirumaran S, Ciattini S (2020) Synthesis, spectral and structural studies on NiS2PN and NiS2P2 chromophores and use of Ni (II) dithiocarbamate to synthesize nickel sulfide and nickel oxide for photodegradation of dyes. J Mol Struct 1220:128704

    Article  CAS  Google Scholar 

  9. Mcyotto F, Wei Q, Macharia DK, Huang M, Shen C, Chow CW (2021) Effect of dye structure on color removal efficiency by coagulation. Chem Eng J 405:126674

    Article  CAS  Google Scholar 

  10. Mashkoor F, Nasar A (2020) Magsorbents: Potential candidates in wastewater treatment technology: a review on the removal of methylene blue dye. J Magn Magn Mater 500:166408

    Article  CAS  Google Scholar 

  11. Coura JC, Profeti D, Profeti LPR (2020) Eco-friendly chitosan/quartzite composite as adsorbent for dye removal. Mater Chem Phys 256:123711

    Article  CAS  Google Scholar 

  12. Elshaarawy RF, Abd El-Azim H, Hegazy WH, Mustafa FH, Talkhan TA (2020) Poly (ammonium/pyridinium)-chitosan Schiff base as a smart biosorbent for scavenging of Cu2+ ions from aqueous effluents. Polym Test 83:106244

    Article  CAS  Google Scholar 

  13. Zheng X, Zheng H, Xiong Z, Zhao R, Liu Y, Zhao C, Zheng C (2020) Novel anionic polyacrylamide-modify-chitosan magnetic composite nanoparticles with excellent adsorption capacity for cationic dyes and pH independent adsorption capability for metal ions. Chem Eng J 392:123706

    Article  CAS  Google Scholar 

  14. Cai W, Zhu F, Liang H, Jiang Y, Tu W, Cai Z, Wu J, Zhou J (2019) Preparation of thiourea-modified magnetic chitosan composite with efficient removal efficiency for Cr (VI). J Chem Eng Data 144:150–158

    CAS  Google Scholar 

  15. Jiang Y, Cai W, Tu W, Zhu M (2019) A facile crosslink method to synthesize magnetic Fe3O4@SiO2-chitosan with high adsorption capacity toward hexavalent chromium. J Chem Eng Data 64(1):226–233

    Article  CAS  Google Scholar 

  16. Li Z, Li L, Hu D, Gao C, Xiong J, Jiang H, Li W (2019) Efficient removal of heavy metal ions and organic dyes with cucurbit [8] uril-functionalized chitosan. J Colloid Interface Sci 539:400–413

    Article  CAS  PubMed  Google Scholar 

  17. Chen Y, Cai W, Dang C, Fan J, Zhou J, Liu Z (2020) A facile sol–gel synthesis of chitosan–boehmite film with excellent acid resistance and adsorption performance for Pb(II). Chem Eng Res Des 161:332–339

    Article  CAS  Google Scholar 

  18. Tanhaei B, Ayati A, Iakovleva E, Sillanpää M (2020) Efficient carbon interlayed magnetic chitosan adsorbent for anionic dye removal: Synthesis, characterization and adsorption study. Int J Biol Macromol 164:3621–3631

    Article  CAS  PubMed  Google Scholar 

  19. Guo M, Wang J, Wang C, Strong PJ, Jiang P, Ok YS, Wang H (2019) Carbon nanotube-grafted chitosan and its adsorption capacity for phenol in aqueous solution. Sci Tot Environ 682:340–347

    Article  CAS  Google Scholar 

  20. Malek NNA, Yousif E, Jawad AH (2020) Optimization of adsorption parameters for reactive red 4 (RR4) removal by cross-linked chitosan-epichlorohydrin using Box Behnken Design. Sci Lett 14(1):83–95

    Google Scholar 

  21. Vithalkar SH, Jugade RM (2020) Adsorptive removal of crystal violet from aqueous solution by cross-linked chitosan coated bentonite. Mater Today Proceed 29:1025–1032

    Article  CAS  Google Scholar 

  22. 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 

  23. Sathiyavimal S, Vasantharaj S, Kaliannan T, Pugazhendhi A (2020) Eco-biocompatibility of chitosan coated biosynthesized copper oxide nanocomposite for enhanced industrial (Azo) dye removal from aqueous solution and antibacterial properties. Carbohydr Polym 241:116243

    Article  CAS  PubMed  Google Scholar 

  24. Ahmad H, Reduan SA, Yusoff N (2018) Nickel oxide nanoparticles grafted with Chitosan as saturable absorber for tunable passively Q-switched fiber laser in S+/S band. Infrared Phys Technol 93:96–102

    Article  CAS  Google Scholar 

  25. Dil EA, Asfaram A, Goudarzi A, Zabihi E, Javadian H (2020) Biocompatible chitosan-zinc oxide nanocomposite based dispersive micro-solid phase extraction coupled with HPLC-UV for the determination of rosmarinic acid in the extracts of medical plants and water sample. Int J Biol Macromol 154:528–537

    Article  CAS  Google Scholar 

  26. Amjadi S, Nazari M, Alizadeh SA, Hamishehkar H (2020) Multifunctional betanin nanoliposomes-incorporated gelatin/chitosan nanofiber/ZnO nanoparticles nanocomposite film for fresh beef preservation. Meat Sci 167:108161

    Article  CAS  PubMed  Google Scholar 

  27. Indumathi MP, Rajarajeswari GR (2019) Mahua oil-based polyurethane/chitosan/nano ZnO composite films for biodegradable food packaging applications. Int J Biol Macromol 124:163–174

    Article  CAS  Google Scholar 

  28. Hassan H, Salama A, El-ziaty AK, El-Sakhawy M (2019) New chitosan/silica/zinc oxide nanocomposite as adsorbent for dye removal. Int J Biol Macromol 131:520–526

    Article  CAS  PubMed  Google Scholar 

  29. Ghaffari SB, Sarrafzadeh MH, Salami M, Khorramizadeh MR (2020) A pH-sensitive delivery system based on N-succinyl chitosan-ZnO nanoparticles for improving antibacterial and anticancer activities of curcumin. Int J Biol Macromol 151:428–440

    Article  CAS  PubMed  Google Scholar 

  30. Hassanein A, Salahuddin N, Matsuda A, Kawamura G, Elfiky M (2017) Fabrication of biosensor based on Chitosan-ZnO/Polypyrrole nanocomposite modified carbon paste electrode for electroanalytical application. Mater Sci Eng C 80:494–501

    Article  CAS  Google Scholar 

  31. Maksoud MA, Elgarahy AM, Farrell C, Ala’a H, Rooney DW, Osman AI (2020) Insight on water remediation application using magnetic nanomaterials and biosorbents. Coord Chem Rev 403:213096

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  33. Garg VK, Kumar R, Gupta R (2004) Removal of malachite green dye from aqueous solution by adsorption using agro-industry waste: a case study of Prosopis cineraria. Dyes Pigm 62(1):1–10

    Article  CAS  Google Scholar 

  34. Soubhagya AS, Moorthi A, Prabaharan M (2020) Preparation and characterization of chitosan/pectin/ZnO porous films for wound healing. Int J Biol Macromol 157:135–145

    Article  CAS  PubMed  Google Scholar 

  35. Motshekga SC, Ray SS, Onyango MS, Momba MN (2015) Preparation and antibacterial activity of chitosan-based nanocomposites containing bentonite-supported silver and zinc oxide nanoparticles for water disinfection. Appl Clay Sci 114:330–339

    Article  CAS  Google Scholar 

  36. 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 

  37. 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 

  38. Mostafa MH, Elsawy MA, Darwish MS, Hussein LI, Abdaleem AH (2020) Microwave-assisted preparation of Chitosan/ZnO nanocomposite and its application in dye removal. Mater Chem Phys 248:122914

    Article  CAS  Google Scholar 

  39. Wang H, Gong X, Miao Y, Guo X, Liu C, Fan YY, Li W (2019) Preparation and characterization of multilayer films composed of chitosan, sodium alginate and carboxymethyl chitosan-ZnO nanoparticles. Food Chem 283:397–403

    Article  CAS  PubMed  Google Scholar 

  40. Malek NNA, Jawad AH, Abdulhameed AS, Ismail K, Hameed BH (2020) New magnetic Schiff’s base-chitosan-glyoxal/fly ash/Fe3O4 biocomposite for the removal of anionic azo dye: An optimized process. Int J Biol Macromol 146:530–539

    Article  PubMed  CAS  Google Scholar 

  41. Rao KM, Suneetha M, Park GT, Babu AG, Han SS (2020) Hemostatic, biocompatible, and antibacterial non-animal fungal mushroom-based carboxymethyl chitosan-ZnO nanocomposite for wound-healing applications. Int J Biol Macromol 155:71–80

    Article  CAS  PubMed  Google Scholar 

  42. 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 

  43. Lingamdinne LP, Koduru JR, Chang YY (2018) Karri Process optimization and adsorption modeling of Pb (II) on nickel ferrite-reduced graphene oxide nano-composite. J Mol Liq 250:202–211

    Article  CAS  Google Scholar 

  44. 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 

  45. Ramlah AB, Jawad AH, Ishak MAM, Kasim NN (2018) FeCl3 -activated carbon developed from coconut leaves: characterization and application for methylene blue removal. Sains Malaysiana 47(3):603–610

    Article  CAS  Google Scholar 

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

    Google Scholar 

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

    Article  CAS  Google Scholar 

  48. 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 

  49. 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 

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

    Google Scholar 

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

    CAS  Google Scholar 

  52. Rizzi V, Gubitosa J, Fini P, Romita R, Agostiano A, Nuzzo S, Cosma P (2020) Commercial bentonite clay as low-cost and recyclable “natural” adsorbent for the Carbendazim removal/recover from water: overview on the adsorption process and preliminary photodegradation considerations. Colloids Surf A Physicochem Eng Asp 602:125060

    Article  CAS  Google Scholar 

  53. Ogunleye DT, Akpotu SO, Moodley B (2020) Adsorption of sulfamethoxazole and reactive blue 19 using graphene oxide modified with imidazolium based ionic liquid. Environ Technol Innov 17:100616

    Article  Google Scholar 

  54. 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 

  55. 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 

  56. 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 

  57. 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 

  58. 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 

  59. 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 

  60. 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 

  61. Zafar MN, Dar Q, Nawaz F, Zafar MN, Iqbal M, Nazar MF (2019) Effective adsorptive removal of azo dyes over spherical ZnO nanoparticles. J Mater Res Technol 8(1):713–725

    Article  CAS  Google Scholar 

  62. Zhang F, Chen X, Wu F, Ji Y (2016) High adsorption capability and selectivity of ZnO nanoparticles for dye removal. Colloids Surf A Physicochem Eng Asp 509:474–483

    Article  CAS  Google Scholar 

  63. 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 

Download references

Acknowledgements

The authors would like to thank the Faculty of Applied Sciences, Universiti Teknologi MARA for facilitating this research work. The sixth and seventh author would like to thank Deanship of Scientific Research, King Saud University for funding through Vice Deanship of Scientific Research Chairs.

Author information

Authors and Affiliations

  1. Laboratory of Molecular Chemistry and Environment, University of Biskra, PO Box 145, Biskra, 07000, Algeria

    Abdallah Reghioua & Djamel Barkat

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

    Abdallah Reghioua & Ali H. Jawad

  3. University of El Oued, Fac. Technology, 39000, El Oued, Algeria

    Abdallah Reghioua

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

    Ahmed Saud Abdulhameed

  5. Department of Biotechnology, School of Chemical and Biotechnology, SASTRA Deemed University, Thanjavur, Tamil Nadu, 613401, India

    S. Rangabhashiyam

  6. Advanced Materials Research Chair, Chemistry Department, College of Science, King Saud University, Riyadh, 11451, Saudi Arabia

    Mohammad Rizwan Khan & Zeid A. ALOthman

Authors
  1. Abdallah Reghioua
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Djamel Barkat
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Ali H. Jawad
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Ahmed Saud Abdulhameed
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. S. Rangabhashiyam
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Mohammad Rizwan Khan
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Zeid A. ALOthman
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Ali H. Jawad.

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

Reghioua, A., Barkat, D., Jawad, A.H. et al. Magnetic Chitosan-Glutaraldehyde/Zinc Oxide/Fe3O4 Nanocomposite: Optimization and Adsorptive Mechanism of Remazol Brilliant Blue R Dye Removal. J Polym Environ 29, 3932–3947 (2021). https://doi.org/10.1007/s10924-021-02160-z

Download citation

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10924-021-02160-z

Keywords

Search

Navigation