Polymer Bulletin

, Volume 76, Issue 2, pp 933–952 | Cite as

Novel nanogels based on hydroxypropyl cellulose–poly(itaconic acid) for adsorption of methylene blue from aqueous solution: process modeling and optimization using response surface methodology

  • Soraya Hassanpour
  • Fahimeh Farshi AzharEmail author
  • Massoumeh BagheriEmail author
Original Paper


The present work studies the adsorptive removal of methylene blue (MB) dye from aqueous solution using a novel biocompatible adsorbent based on hydroxypropyl cellulose (HPC) and itaconic acid nanogels. The biocompatible adsorbent was characterized using scanning electron microscopy, Fourier transform infrared spectroscopy and dynamic light scattering analyses. Response surface methodology was used to modeling and optimization of the adsorption process. A second-order empirical relationship between adsorption capacity and independent variables (pH of the solution, contact time and dye concentration) was obtained. The results of design of experiments demonstrated that the predicted values were well fitted with the experimental data where coefficient of determination (R2) equaled 0.9861. Pareto analysis for identification of the factors effect on the system revealed that the initial concentration of MB was the most effective parameter. Maximum removal efficiency (99.9%) was achieved at optimum parameters where pH, MB concentration, and contact time were 5.6, 130 mg L−1, and 5 min, respectively. Furthermore, the adsorption experimental data were well fitted to the Temkin isotherm and pseudo-second-order kinetic model. Consequently, it was found out that the HPC–PIA nanogels with high adsorption capacity (nearly 761 mg g−1) can be a suitable adsorbent for removal of cationic dyes from textile colored wastewaters.


Nanogel Hydroxypropyl cellulose Itaconic acid Methylene blue Adsorption Response surface methodology 



We thank the Vice Chancellor of Research of Azarbaijan Shahid Madani University, for financially supporting this research.


  1. 1.
    Entezari M, Al-Hoseini ZS, Ashraf N (2008) Fast and efficient removal of reactive black 5 from aqueous solution by a combined method of ultrasound and sorption process. Ultrason Sonochem 15(4):433–437Google Scholar
  2. 2.
    Gong R, Li M, Yang C, Sun Y, Chen J (2005) Removal of cationic dyes from aqueous solution by adsorption on peanut hull. J Hazard Mater 121(1):247–250Google Scholar
  3. 3.
    Mahida VP, Patel MP (2016) Removal of some most hazardous cationic dyes using novel poly (NIPAAm/AA/N-allylisatin) nanohydrogel. Arab J Chem 9(3):430–442Google Scholar
  4. 4.
    Rahman MM, Choudhury FA, Hossain MD, Chowdhury MNI, Mohsin S, Hasan MM, Uddin MF, Sarker NC (2014) A Comparative study on the photocatalytic degradation of industrial dyes using modified commercial and synthesized TiO2 photocatalysts. J Chem Eng 27(2):65–71Google Scholar
  5. 5.
    Zollinger H (2003) Color chemistry: syntheses, properties, and applications of organic dyes and pigments. Wiley, LondonGoogle Scholar
  6. 6.
    Habibi MH, Hassanzadeh A, Mahdavi S (2005) The effect of operational parameters on the photocatalytic degradation of three textile azo dyes in aqueous TiO2 suspensions. J Photochem Photobiol A Chem 172(1):89–96Google Scholar
  7. 7.
    Hakam A, Rahman IA, Jamil MSM, Othaman R, Amin MCIM, Lazim MASM (2015) Removal of methylene blue dye in aqueous solution by sorption on a bacterial-g-poly-(acrylic acid) polymer network hydrogel. Sains Malays 44(6):827–834Google Scholar
  8. 8.
    Frankenburg FR, Baldessarini RJ (2008) Neurosyphilis, malaria, and the discovery of antipsychotic agents. Harvard Rev Psychiatry 16(5):299–307Google Scholar
  9. 9.
    Oz M, Lorke DE, Petroianu GA (2009) Methylene blue and Alzheimer’s disease. Biochem Pharmacol 78(8):927–932Google Scholar
  10. 10.
    Lin S, Lo C (1996) Treatment of textile wastewater by foam flotation. Environ Technol 17(8):841–849Google Scholar
  11. 11.
    Tahir S, Rauf N (2006) Removal of a cationic dye from aqueous solutions by adsorption onto bentonite clay. Chemosphere 63(11):1842–1848Google Scholar
  12. 12.
    Qiu H, Lv L, Pan B-c, Zhang Q-j, Zhang W-m, Zhang Q-x (2009) Critical review in adsorption kinetic models. J Zhejiang Univ Sci A 10(5):716–724Google Scholar
  13. 13.
    Carmen Z, Daniela S (2012) Textile organic dyes-characteristics, polluting effects and separation/elimination procedures from industrial effluents—a critical overview. In: Puzyn T (ed) Organic pollutants ten years after the stockholm convention-environmental and analytical update. InTech, Croatia, pp 55–81Google Scholar
  14. 14.
    Wen X, Qiao X, Han X, Niu L, Huo L, Bai G (2016) Multifunctional magnetic branched polyethylenimine nanogels with in situ generated Fe3O4 and their applications as dye adsorbent and catalyst support. J Mater Sci 51(6):3170–3181Google Scholar
  15. 15.
    Zhang X, Malhotra S, Molina M, Haag R (2015) Micro-and nanogels with labile crosslinks—from synthesis to biomedical applications. Chem Soc Rev 44(7):1948–1973Google Scholar
  16. 16.
    Koetting MC, Peters JT, Steichen SD, Peppas NA (2015) Stimulus-responsive hydrogels: theory, modern advances, and applications. Mater Sci Eng R Rep 93:1–49Google Scholar
  17. 17.
    Sharma A, Garg T, Aman A, Panchal K, Sharma R, Kumar S, Markandeywar T (2016) Nanogel-an advanced drug delivery tool: current and future. Artif Cells Nanomed Biotechnol 44(1):165–177Google Scholar
  18. 18.
    Honarkar H, Barikani M (2009) Applications of biopolymers I: chitosan. Monatsh Chem Chem Mon 140(12):1403Google Scholar
  19. 19.
    Hu D, Wang P, Ma Q, Wang L (2016) Preparation of a cellulose-based adsorbent with covalently attached hydroxypropyl dodecyldimethylammonium groups for the removal of CI Reactive Blue 21 dye from aqueous solution. Desalin Water Treat 57(23):10604–10615Google Scholar
  20. 20.
    Üzüm ÖB, Karadağ E (2011) Dye sorption and water uptake properties of crosslinked acrylamide/sodium methacrylate copolymers and semi-interpenetrating polymer networks composed of PEG. Sep Sci Technol 46(3):489–499Google Scholar
  21. 21.
    Wang R, Yu B, Jiang X, Yin J (2012) Understanding the host-guest interaction between responsive core-crosslinked hybrid nanoparticles of hyperbranched poly (ether amine) and dyes: the selective adsorption and smart separation of dyes in water. Adv Funct Mater 22(12):2606–2616Google Scholar
  22. 22.
    Hoshino Y, Imamura K, Yue M, Inoue G, Miura Y (2012) Reversible absorption of CO2 triggered by phase transition of amine-containing micro-and nanogel particles. J Am Chem Soc 134(44):18177–18180Google Scholar
  23. 23.
    Atta A, Akl MA, Youssef AM, Ibraheim MA (2013) Superparamagnetic core-shell polymeric nanocomposites for efficient removal of methylene blue from aqueous solutions. Adsorpt Sci Technol 31(5):397–419Google Scholar
  24. 24.
    Akl MA, Sarhan AA, Shoueir KR, Atta AM (2013) Application of crosslinked ionic poly (vinyl alcohol) nanogel as adsorbents for water treatment. J Dispers Sci Technol 34(10):1399–1408Google Scholar
  25. 25.
    Lakouraj MM, Mojerlou F, Zare EN (2014) Nanogel and superparamagnetic nanocomposite based on sodium alginate for sorption of heavy metal ions. Carbohyd Polym 106:34–41Google Scholar
  26. 26.
    Chatterjee S, Kumar A, Basu S, Dutta S (2012) Application of response surface methodology for methylene blue dye removal from aqueous solution using low cost adsorbent. Chem Eng J 181:289–299Google Scholar
  27. 27.
    Dutta S, Bhattacharyya A, Ganguly A, Gupta S, Basu S (2011) Application of response surface methodology for preparation of low-cost adsorbent from citrus fruit peel and for removal of methylene blue. Desalination 275(1):26–36Google Scholar
  28. 28.
    Jahangiri M, Bagheri M, Farshi F, Abbasi F (2015) Optimized synthesis of hydroxypropyl cellulose-g-poly (ε-caprolactone) network. J Poly Res 22(10):1–13Google Scholar
  29. 29.
    Olad A, Farshi Azhar F, Shargh M, Jharfi S (2014) Application of response surface methodology for modeling of reactive dye removal from solution using starch-montmorillonite/polyaniline nanocomposite. Polym Eng Sci 54(7):1595–1607Google Scholar
  30. 30.
    Silva JP, Sousa S, Gonçalves I, Porter JJ, Ferreira-Dias S (2004) Modelling adsorption of acid orange 7 dye in aqueous solutions to spent brewery grains. Sep Purif Technol 40(2):163–170Google Scholar
  31. 31.
    Qiu X, Hu S (2013) “Smart” materials based on cellulose: a review of the preparations, properties, and applications. Materials 6(3):738–781Google Scholar
  32. 32.
    Pulat M, Eksi H (2006) Determination of swelling behavior and morphological properties of poly (acrylamide-co-itaconic acid) and poly (acrylic acid-co-itaconic acid) copolymeric hydrogels. J Appl Polym Sci 102(6):5994–5999Google Scholar
  33. 33.
    Betancourt T, Pardo J, Soo K, Peppas NA (2010) Characterization of pH-responsive hydrogels of poly (itaconic acid-g-ethylene glycol) prepared by UV-initiated free radical polymerization as biomaterials for oral delivery of bioactive agents. J Biomed Mater Res A 93(1):175–188Google Scholar
  34. 34.
    Hassanpour S, Bagheri M (2017) Dual-responsive semi-IPN copolymer nanogels based on poly (itaconic acid) and hydroxypropyl cellulose as a carrier for controlled drug release. J Polym Res 24(6):91Google Scholar
  35. 35.
    Liang C, Rogers C, Malafeew E (1997) Investigation of shape memory polymers and their hybrid composites. J Intell Mater Syst Struct 8(4):380–386Google Scholar
  36. 36.
    Özcan A, Ömeroğlu Ç, Erdoğan Y, Özcan AS (2007) Modification of bentonite with a cationic surfactant: an adsorption study of textile dye reactive blue 19. J Hazard Mater 140(1):173–179Google Scholar
  37. 37.
    Ma L, Kang H, Liu R, Huang Y (2010) Smart assembly behaviors of hydroxypropyl cellulose-graft-poly (4-vinyl pyridine) copolymers in aqueous solution by thermo and pH stimuli. Langmuir 26(23):18519–18525Google Scholar
  38. 38.
    Miller JN, Miller JC (2005) Statistics and chemometrics for analytical chemistry. Pearson Education, New YorkGoogle Scholar
  39. 39.
    Moghaddam SS, Alavi Moghaddam MR, Arami M (2012) Response surface optimization of acid red 119 dye adsorption by mixtures of dried sewage sludge and sewage sludge ash. Clean Soil Air Water 40(6):652–660Google Scholar
  40. 40.
    Zhu H-Y, Fu Y-Q, Jiang R, Yao J, Xiao L, Zeng G-M (2012) Novel magnetic chitosan/poly (vinyl alcohol) hydrogel beads: preparation, characterization and application for adsorption of dye from aqueous solution. Bioresour Technol 105:24–30Google Scholar
  41. 41.
    Pandey S, Mishra SB (2011) Organic–inorganic hybrid of chitosan/organoclay bionanocomposites for hexavalent chromium uptake. J Colloid Interface Sci 361(2):509–520Google Scholar
  42. 42.
    Gimbert F, Morin-Crini N, Renault F, Badot P-M, Crini G (2008) Adsorption isotherm models for dye removal by cationized starch-based material in a single component system: error analysis. J Hazard Mater 157(1):34–46Google Scholar
  43. 43.
    Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40(9):1361–1403Google Scholar
  44. 44.
    Freundlich H (1906) Over the adsorption in solution. J Phys Chem 57(385471):1100–1107Google Scholar
  45. 45.
    Hameed B, Tan I, Ahmad A (2008) Optimization of basic dye removal by oil palm fibre-based activated carbon using response surface methodology. J Hazard Mater 158(2):324–332Google Scholar
  46. 46.
    Bayramoglu G, Altintas B, Arica MY (2009) Adsorption kinetics and thermodynamic parameters of cationic dyes from aqueous solutions by using a new strong cation-exchange resin. Chem Eng J 152(2):339–346Google Scholar
  47. 47.
    Tempkin M, Pyzhev V (1940) Kinetics of ammonia synthesis on promoted iron catalyst. Acta Phys Chim USSR 12(1):327Google Scholar
  48. 48.
    Auta M, Hameed B (2011) Optimized waste tea activated carbon for adsorption of methylene blue and acid blue 29 dyes using response surface methodology. Chem Eng J 175:233–243Google Scholar
  49. 49.
    Roosta M, Ghaedi M, Daneshfar A, Sahraei R, Asghari A (2014) Optimization of the ultrasonic assisted removal of methylene blue by gold nanoparticles loaded on activated carbon using experimental design methodology. Ultrason Sonochem 21(1):242–252Google Scholar
  50. 50.
    Tehrani MS, Zare-Dorabei R (2016) Competitive removal of hazardous dyes from aqueous solution by MIL-68 (Al): derivative spectrophotometric method and response surface methodology approach. Acta A Mol Biomol Spectrosc 160:8–18Google Scholar
  51. 51.
    Ghaedi M, Pakniat M, Mahmoudi Z, Hajati S, Sahraei R, Daneshfar A (2014) Synthesis of nickel sulfide nanoparticles loaded on activated carbon as a novel adsorbent for the competitive removal of methylene blue and safranin-O. Spectrochim Acta A Mol Biomol Spectrosc 123:402–409Google Scholar
  52. 52.
    Sadhukhan B, Mondal NK, Chattoraj S (2016) Optimisation using central composite design (CCD) and the desirability function for sorption of methylene blue from aqueous solution onto Lemna major. Karbala Int J Mod Sci 2(3):145–155Google Scholar
  53. 53.
    Ghaedi M, Ghazanfarkhani MD, Khodadoust S, Sohrabi N, Oftade M (2014) Acceleration of methylene blue adsorption onto activated carbon prepared from dross licorice by ultrasonic: equilibrium, kinetic and thermodynamic studies. J Ind Eng Chem 20(4):2548–2560Google Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Chemistry Department, Science FacultyAzarbaijan Shahid Madani UniversityTabrizIran

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