Skip to main content
Log in

Facile preparation of three-dimensional graphene oxide/ \({\iota}\)-carrageenan composite aerogel and its efficient ability for selective adsorption of methylene blue

  • Polymers & biopolymers
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

A three-dimensional graphene oxide/\({\iota}\)-carrageenan composite aerogel (GO/\({\iota}\)-Car) has been facilely manufactured in a benign approach and characterized in detail. The adsorption ability of the GO/ \({\iota}\)-Car aerogel was also investigated on the methylene blue (MB) removal from synthesized solutions. It was found that the adsorption process followed the pseudo-second-order kinetic model. The Langmuir maximum adsorption capacity of MB on the GO/\({\iota}\)-Car aerogel was calculated to be 245.28 mg g−1. Thermodynamic calculations proved that the adsorption was a spontaneous, exothermic process with the enthalpy change of −10.36 kJ mol−1 and the entropy change of 54.64 J mol−1 K−1. Furthermore, adsorption selectivity studies showed that the GO/ \({\iota}\)-Car aerogel could selectively adsorb the cationic MB in the presence of anionic dye methyl orange, which was mainly attributed to the electrostatic attraction between the negatively charged aerogel and the positively charged MB. In addition, the MB removal rate by the GO/\({\iota}\)-Car aerogel could still reach 91.9% after three desorption–adsorption cycles. Overall, the GO/\({\iota}\)-Car aerogel prepared in this study could be a green, cost-effective, reusable and promising selective adsorbent for cationic dye removal from water.

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

Access this article

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

Instant access to the full article PDF.

Scheme 1
Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7
Figure 8
Figure 9
Figure 10
Figure 11

Similar content being viewed by others

References

  1. Xu H, Yang B, Liu Y, Li F, Shen C, Ma C, Tian Q, Song X, Sand W (2018) Recent advances in anaerobic biological processes for textile printing and dyeing wastewater treatment: a mini-review. World J Microbiol Biotechnol 34:165

    Article  Google Scholar 

  2. Manna S, Roy D, Saha P, Gopakumar D, Thomas S (2017) Rapid methylene blue adsorption using modified lignocellulosic materials. Process Saf Environ 107:346–356

    Article  CAS  Google Scholar 

  3. Alvarez MS, Moscoso F, Rodriguez A, Sanroman MA, Deive FJ (2013) Novel physico-biological treatment for the remediation of textile dyes-containing industrial effluents. Bioresour Technol 146:689–695

    Article  CAS  Google Scholar 

  4. Verma AK, Dash RR, Bhunia P (2012) A review on chemical coagulation/flocculation technologies for removal of colour from textile wastewaters. J Environ Manage 93:154–168

    Article  CAS  Google Scholar 

  5. Wang J, Wu Z, Li T, Ye J, Shen L, She Z, Liu F (2018) Catalytic PVDF membrane for continuous reduction and separation of p-nitrophenol and methylene blue in emulsified oil solution. Chem Eng J 334:579–586

    Article  CAS  Google Scholar 

  6. Li B, Dong Y, Zou C, Xu Y (2014) Iron (III)-alginate fiber complex as a highly effective and stable heterogeneous fenton photocatalyst for mineralization of organic dye. Ind Eng Chem Res 53:4199–4206

    Article  CAS  Google Scholar 

  7. Pethsangave DA, Khose RV, Wadekar PH, Kulal DK, Some S (2020) One-Pot synthetic approach for magnetically separable graphene nanocomposite for dye degradation. ChemistrySelect 5:1516–1525

    Article  CAS  Google Scholar 

  8. Li L, Qi G, Wang B, Yue D, Wang Y, Sato T (2018) Fulvic acid anchored layered double hydroxides: a multifunctional composite adsorbent for the removal of anionic dye and toxic metal. J Hazard Mater 343:19–28

    Article  CAS  Google Scholar 

  9. Zbair M, Anfar Z, Khallok H, Ahsaine HA, Ezahri M, Elalem N (2018) Adsorption kinetics and surface modeling of aqueous methylene blue onto activated carbonaceous wood sawdust. Fuller Nanotub Car N 26:433–442

    Article  CAS  Google Scholar 

  10. Hosseini SM, Shahrousvand M, Shojaei S, Khonakdar HA, Asefnejad A, Goodarzi V (2020) Preparation of superabsorbent eco-friendly semi-interpenetrating network based on cross-linked poly acrylic acid/xanthan gum/graphene oxide (PAA/XG/GO): characterization and dye removal ability. Int J Biol Macromol 152:884–893

    Article  CAS  Google Scholar 

  11. Zhou Y, Lu J, Zhou Y, Liu Y (2019) Recent advances for dyes removal using novel adsorbents: a review. Environ Pollut 252:352–365

    Article  CAS  Google Scholar 

  12. Zambare R, Song X, Bhuvana S, Antony Prince JS, Nemade P (2017) Ultrafast dye removal using ionic liquid-graphene oxide sponge. ACS Sustain Chem Eng 5:6026–6035

    Article  CAS  Google Scholar 

  13. Hu K, Xie X, Szkopek T, Cerruti M (2016) Understanding hydrothermally reduced graphene oxide hydrogels: from reaction products to hydrogel properties. Chem Mater 28:1756–1768

    Article  CAS  Google Scholar 

  14. Song S, Ma Y, Shen H, Zhang M, Zhang Z (2015) Removal and recycling of ppm levels of methylene blue from an aqueous solution with graphene oxide. RSC Adv 5:27922–27932

    Article  CAS  Google Scholar 

  15. Sitko R, Turek E, Zawisza B, Malicka E, Talik E, Heimann J, Gagor A, Feist B, Wrzalik R (2013) Adsorption of divalent metal ions from aqueous solutions using graphene oxide. Dalton Trans 42:5682–5689

    Article  CAS  Google Scholar 

  16. Boukhalfa N, Boutahala M, Djebri N, Idris A (2019) Kinetics, thermodynamics, equilibrium isotherms, and reusability studies of cationic dye adsorption by magnetic alginate/oxidized multiwalled carbon nanotubes composites. Int J Biol Macromol 123:539–548

    Article  CAS  Google Scholar 

  17. Yang X, Li Y, Du Q, Sun J, Chen L, Hu S, Wang Z, Xia Y, Xia L (2015) Highly effective removal of basic fuchsin from aqueous solutions by anionic polyacrylamide/graphene oxide aerogels. J Colloid Interface Sci 453:107–114

    Article  CAS  Google Scholar 

  18. Chen L, Li Y, Du Q, Wang Z, Xia Y, Yedinak E, Lou J, Ci L (2017) High performance agar/graphene oxide composite aerogel for methylene blue removal. Carbohydr Polym 155:345–353

    Article  CAS  Google Scholar 

  19. Yan M, Huang W, Li Z (2019) Chitosan cross-linked graphene oxide/lignosulfonate composite aerogel for enhanced adsorption of methylene blue in water. Int J Biol Macromol 136:927–935

    Article  CAS  Google Scholar 

  20. Sashkina KA, Gurikov PA, Ayupov AB, Smirnova I, Parkhomchuk EV (2018) Zeolite/silica aerogel composite monoliths and microspheres. Micropor Mesopor Mat 263:106–112

    Article  CAS  Google Scholar 

  21. Daniel-da-Silva AL, Salgueiro AM, Creaney B, Oliveira-Silva R, Silva NJO, Trindade T (2015) Carrageenan-grafted magnetite nanoparticles as recyclable sorbents for dye removal. J Nanopart Res 17:302

    Article  Google Scholar 

  22. Soedjak HS (2002) Colorimetric determination of carrageenans and other anionic hydrocolloids with methylene blue. Anal Chem 66:4514–4518

    Article  Google Scholar 

  23. Liu C, Omer AM, Ouyang XK (2018) Adsorptive removal of cationic methylene blue dye using carboxymethyl cellulose/κ-carrageenan/activated montmorillonite composite beads: Isotherm and kinetic studies. Int J Biol Macromol 106:823–833

    Article  CAS  Google Scholar 

  24. Duman O, Tunc S, Polat TG, Bozoglan BK (2016) Synthesis of magnetic oxidized multiwalled carbon nanotube-kappa-carrageenan-Fe3O4 nanocomposite adsorbent and its application in cationic Methylene Blue dye adsorption. Carbohydr Polym 147:79–88

    Article  CAS  Google Scholar 

  25. Qu W, He D, Huang H, Guo Y, Tang Y, Song R (2020) Characterization of amino-crosslinked hypromellose and its adsorption characteristics for methyl orange from water. J Mater Sci 55:7268–7282. https://doi.org/10.1007/s10853-020-04517-6

    Article  CAS  Google Scholar 

  26. Pu W, Song Z, Yan J, Xu H, Ji H, Yuan S, Li H (2019) Preparation of oxygen-deficient 2D WO3-x nanoplates and their adsorption behaviors for organic pollutants: equilibrium and kinetics modeling. J Mater Sci 54:12463–12475

    Article  CAS  Google Scholar 

  27. Ersan G, Kaya Y, Ersan MS, Apul OG, Karanfil T (2019) Adsorption kinetics and aggregation for three classes of carbonaceous adsorbents in the presence of natural organic matter. Chemosphere 229:515–524

    Article  CAS  Google Scholar 

  28. 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 

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

    CAS  Google Scholar 

  30. Abdulla NK, Siddiqui SI, Tara N, Hashmi AA, Chaudhry SA (2019) Psidium guajava leave-based magnetic nanocomposite γ-Fe2O3@GL: a green technology for methylene blue removal from water. J Environ Chem Eng 7:103423

    Article  CAS  Google Scholar 

  31. Tran HN, You SJ, Hosseini-Bandegharaei A, Chao HP (2017) Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions: a critical review. Water Res 120:88–116

    Article  CAS  Google Scholar 

  32. Yang ST, Chang Y, Wang H, Liu G, Chen S, Wang Y, Liu Y, Cao A (2010) Folding/aggregation of graphene oxide and its application in Cu2+ removal. J Colloid Interface Sci 351:122–127

    Article  CAS  Google Scholar 

  33. Morimune S, Nishino T, Goto T (2012) Poly (vinyl alcohol)/graphene oxide nanocomposites prepared by a simple eco-process. Polym J 44:1056–1063

    Article  CAS  Google Scholar 

  34. Paşcalău V, Popescu V, Popescu GL, Dudescu MC, Borodi G, Dinescu A, Perhaiţa I, Paul M (2012) The alginate/κ-carrageenan ratio’s influence on the properties of the cross-linked composite films. J Alloy Compd 536:S418–S423

    Article  Google Scholar 

  35. Nanaki S, Karavas E, Kalantzi L, Bikiaris D (2010) Miscibility study of carrageenan blends and evaluation of their effectiveness as sustained release carriers. Carbohydr Polym 79:1157–1167

    Article  CAS  Google Scholar 

  36. Rasool N, Yasin T, Heng JYY, Akhter Z (2010) Synthesis and characterization of novel pH-, ionic strength and temperature-sensitive hydrogel for insulin delivery. Polymer 51:1687–1693

    Article  CAS  Google Scholar 

  37. Prado-Fernández J, Rodriguez-Vazquez JA, Tojo E, Andrade JM (2003) Quantitation of κ-, ι- and λ-carrageenans by mid-infrared spectroscopy and PLS regression. Analytica Chimica Acta 480:23–37

    Article  Google Scholar 

  38. Wu Z, Huang W, Shan X, Li Z (2020) Preparation of a porous graphene oxide/alkali lignin aerogel composite and its adsorption properties for methylene blue. Int J Biol Macromol 143:325–333

    Article  CAS  Google Scholar 

  39. Lokhande KD, Pethsangave DA, Kulal DK, Some S (2020) Remediation of toxic dye pollutants by using graphene-based adsorbents. Chem Select 5:8062–8073

    CAS  Google Scholar 

  40. Zhang D-D, Zu S-Z, Han B-H (2009) Inorganic-organic hybrid porous materials based on graphite oxide sheets. Carbon 47:2993–3000

    Article  CAS  Google Scholar 

  41. Kong Y, Wang L, Ge Y, Su H, Li Z (2019) Lignin xanthate resin-bentonite clay composite as a highly effective and low-cost adsorbent for the removal of doxycycline hydrochloride antibiotic and mercury ions in water. J Hazard Mater 368:33–41

    Article  CAS  Google Scholar 

  42. Prasad K, Kaneko Y, Kadokawa J (2009) Novel gelling systems of kappa-, iota- and lambda-carrageenans and their composite gels with cellulose using ionic liquid. Macromol Biosci 9:376–382

    Article  CAS  Google Scholar 

  43. Wang J, Zhao G, Jing L, Peng X, Li Y (2015) Facile self-assembly of magnetite nanoparticles on three-dimensional graphene oxide-chitosan composite for lipase immobilization. Biochem Eng J 98:75–83

    Article  CAS  Google Scholar 

  44. Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y, Wu Y, Nguyen ST, Ruoff RS (2007) Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45:1558–1565

    Article  CAS  Google Scholar 

  45. Qi Y, Yang M, Xu W, He S, Men Y (2017) Natural polysaccharides-modified graphene oxide for adsorption of organic dyes from aqueous solutions. J Colloid Interface Sci 486:84–96

    Article  CAS  Google Scholar 

  46. Inbaraj BS, Chen BH (2011) Dye adsorption characteristics of magnetite nanoparticles coated with a biopolymer poly (gamma-glutamic acid). Bioresour Technol 102:8868–8876

    Article  Google Scholar 

  47. Rocher V, Bee A, Siaugue JM, Cabuil V (2010) Dye removal from aqueous solution by magnetic alginate beads crosslinked with epichlorohydrin. J Hazard Mater 178:434–439

    Article  CAS  Google Scholar 

  48. Qin L, Ge Y, Deng B, Li Z (2017) Poly (ethylene imine) anchored lignin composite for heavy metals capturing in water. J Taiwan Inst Chem E 71:84–90

    Article  CAS  Google Scholar 

  49. Abdellah AR, Abdelhamid HN, El-Adasy A-BAAM, Atalla AA, Aly KI (2020) One-pot synthesis of hierarchical porous covalent organic frameworks and two-dimensional nanomaterials for selective removal of anionic dyes. J Environ Chem Eng 8:104054

    Article  CAS  Google Scholar 

  50. Liu Y, Luo C, Sun J, Li H, Sun Z, Yan S (2015) Enhanced adsorption removal of methyl orange from aqueous solution by nanostructured proton-containing δ-MnO2. J Mater Chem A 3:5674–5682

    Article  CAS  Google Scholar 

  51. Ho YS (2006) Review of second-order models for adsorption systems. J Hazard Mater 136:681–689

    Article  CAS  Google Scholar 

  52. Tang S, Xia D, Yao Y, Chen T, Sun J, Yin Y, Shen W, Peng Y (2019) Dye adsorption by self-recoverable, adjustable amphiphilic graphene aerogel. J Colloid Interface Sci 554:682–691

    Article  CAS  Google Scholar 

  53. Zhang F, Xue X, Huang X, Yang H (2020) Adsorption and heterogeneous Fenton catalytic performance for magnetic Fe3O4/reduced graphene oxide aerogel. J Mater Sci 55:15695–15708

    Article  CAS  Google Scholar 

  54. Kaur K, Jindal R, Meenu (2019) Self-assembled GO incorporated CMC and Chitosan-based nanocomposites in the removal of cationic dyes. Carbohydr Polym 225:115245

    Article  CAS  Google Scholar 

  55. Ren F, Li Z, Tan WZ, Liu XH, Sun ZF, Ren PG, Yan DX (2018) Facile preparation of 3D regenerated cellulose/graphene oxide composite aerogel with high-efficiency adsorption towards methylene blue. J Colloid Interface Sci 532:58–67

    Article  CAS  Google Scholar 

  56. Liu J, Chu H, Wei H, Zhu H, Wang G, Zhu J, He J (2016) Facile fabrication of carboxymethyl cellulose sodium/graphene oxide hydrogel microparticles for water purification. RSC Adv 6:50061–50069

    Article  CAS  Google Scholar 

  57. Dai H, Zhang Y, Ma L, Zhang H, Huang H (2019) Synthesis and response of pineapple peel carboxymethyl cellulose-g-poly (acrylic acid-co-acrylamide)/graphene oxide hydrogels. Carbohydr Polym 215:366–376

    Article  CAS  Google Scholar 

  58. Eltaweil AS, Elgarhy GS, El-Subruiti GM, Omer AM (2020) Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads for efficient adsorption of cationic methylene blue dye. Int J Biol Macromol 154:307–318

    Article  CAS  Google Scholar 

  59. Teli MD, Nadathur GT (2018) Adsorptive removal of acid yellow 17 (an anionic dye) from water by novel ionene chloride modified electrospun silica nanofibres. J Environ Chem Eng 6:7257–7272

    Article  CAS  Google Scholar 

  60. Dai J, Xie A, Zhang R, Ge W, Chang Z, Tian S, Li C, Yan Y (2018) Scalable preparation of hierarchical porous carbon from lignin for highly efficient adsorptive removal of sulfamethazine antibiotic. J Mol Liq 256:203–212

    Article  CAS  Google Scholar 

  61. Saxena R, Saxena M, Lochab A (2020) Recent progress in nanomaterials for adsorptive removal of organic contaminants from wastewater. Chem Select 5:335–353

    CAS  Google Scholar 

  62. Dai L, Zhu W, He L, Tan F, Zhu N, Zhou Q, He M, Hu G (2018) Calcium-rich biochar from crab shell: An unexpected super adsorbent for dye removal. Bioresour Technol 267:510–516

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was financially supported by the Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science (20180510004) and the National Natural Science Foundation of China (51479016, 51908409).

Author information

Authors and Affiliations

Authors

Contributions

GS was involved in methodology, data curation, investigation and writing—original draft. YS was involved in writing—review and editing. AL was involved in formal analysis and data curation. HW was involved in investigation, visualization and formal analysis. GD was involved in writing—review and editing, conceptualization, resources and supervision.

Corresponding author

Correspondence to Guanghui Ding.

Ethics declarations

Conflict of interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Additional information

Handling Editor: Lisa White.

Publisher's Note

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

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 1878 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Song, G., Shi, Y., Li, A. et al. Facile preparation of three-dimensional graphene oxide/ \({\iota}\)-carrageenan composite aerogel and its efficient ability for selective adsorption of methylene blue. J Mater Sci 56, 14866–14879 (2021). https://doi.org/10.1007/s10853-021-06211-7

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-021-06211-7

Navigation