Polymer Bulletin

, Volume 75, Issue 9, pp 3825–3841 | Cite as

A comparative study between three different methods of hydrogel network characterization: effect of composition on the crosslinking properties using sol–gel, rheological and mechanical analyses

  • Nour Elhouda Ben AmmarEmail author
  • Taib Saied
  • Mohamed Barbouche
  • Faouzi Hosni
  • Ahmed Hichem Hamzaoui
  • Murat Şen
Original Paper


Previously, different techniques were used to identify the crosslinking density of hydrogels. In this study, we aimed to compare three different methods of network structure determination: using sol–gel analyses, rheological and mechanical experiments. To do this, we synthesized a polyvinylpyrrolidone (PVP) hydrogel using gamma-ray crosslinking. The effect of dose, PVP, polyethylene glycol (PEG) and agar content on network properties and mesh size were investigated. It was found that rheological experiment gives more precise results. Determined network parameters such as molecular weight between crosslinks \(\left( {\overline{{M_{\text{c}} }} } \right)\), crosslinking density (v e) and mesh size (ξ), were used to determine the impact of composition on physicochemical properties. It was found that increasing dose and PVP content leads to an increase in the crosslinking density and a decrease in pore size. However, increasing agar and PEG molar ratio leads to a decrease in the crosslinking density. Regarding elastic behavior, it was found that agar increases viscous modulus and acts as a crosslinking inhibitor but PEG decreases it and acts as a plasticizer. These results were confirmed by determining the state of water in hydrogel network using pulse NMR. SEM images confirmed also calculated network parameters.


Crosslink density Hydrogel Network Pulse NMR 


Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.


  1. 1.
    Jones DS (1999) Dynamic mechanical analysis of polymeric systems of pharmaceutical and biomedical significance. Int J Pharm 179:167–178CrossRefPubMedGoogle Scholar
  2. 2.
    Fechine GJM, Barros JAG, Alcântara MR, Catalani LH (2006) Fluorescence polarization and rheological studies of the poly(N-vinyl-2-pyrrolidone) hydrogels produced by UV radiation. Polymer 47:2629–2633CrossRefGoogle Scholar
  3. 3.
    Şen M, Hayrabolulu H (2012) Radiation synthesis and characterisation of the network structure of natural/synthetic double-network superabsorbent polymers. Radiat Phys Chem 81:1378–1382CrossRefGoogle Scholar
  4. 4.
    Enas MA (2015) Hydrogel: preparation, characterization, and applications: a review. J Adv Res 6:105–121CrossRefGoogle Scholar
  5. 5.
    Maolin Z, Jun L, Min Y, Hongfei H (2000) The swelling behaviour of radiation prepared semi-interpenetrating polymer networks composed of polyNIPAAm and hydrophilic polymers. Radiat Phys Chem 58:397–400CrossRefGoogle Scholar
  6. 6.
    Rosiak JM, Ulanski P (1999) Synthesis of hydrogels by irradiation of polymers in aqueous solution. Radiat Phys Chem 55:139CrossRefGoogle Scholar
  7. 7.
    Momesso RGRAP, Moreno CS, Rogero SO, Rogero JR, Spencer PJ, Lugão AB (2010) Radiation stability of resveratrol in immobilization on poly vinyl pyrrolidone hydrogel dressing for dermatological use. Radiat Phys Chem 79:283–285CrossRefGoogle Scholar
  8. 8.
    Rosiak JM, Olejniczak J, Pȩkala W (1990) Fast reaction of irradiated polymers crosslinking and degradation of polyvinylpyrrolidone. Radiat Phys Chem 36:747–755Google Scholar
  9. 9.
    Ajji Z, Mirjalili G, Alkhatab A, Dada H (2008) Use of electron beam for the production of hydrogel dressings. Radiat Phys Chem 77:200–202CrossRefGoogle Scholar
  10. 10.
    Lilian C, Lopérgolo B, Ademar L, Catalani H (2003) Direct UV photocrosslinking of poly(N-vinyl-2-pyrrolidone) (PVP) to produce hydrogels. Polymer 44:6217–6222CrossRefGoogle Scholar
  11. 11.
    Lugao AB, Sizue O, Malmonge RS (2002) Rheological behaviour of irradiated wound dressing poly(vinyl pyrrolidone) hydrogels. Radiat Phys Chem 63:543–546CrossRefGoogle Scholar
  12. 12.
    Farah K, Jerbi T, Kuntz F, Kovacs A (2006) Dose measurements for characterization of a semi-industrial cobalt-60 gamma-irradiation facility. Radiat Measur 41:201–208CrossRefGoogle Scholar
  13. 13.
    Mark JE, Erman B (1988) Rubberlike elasticity a molecular primer, 2nd edn. Wiley, NewYorkGoogle Scholar
  14. 14.
    Mahmudi N, Sen M, Rendevski S, Guven O (2007) Radiation synthesis of low swelling acrylamide based hydrogels and determination of average molecular weight between crosslinks. Nucl Instr Methods Phys Res B 265:375–378CrossRefGoogle Scholar
  15. 15.
    Sen M, Yakar A, Guven O (1999) Determination of average molecular weight between crosslinks from swelling behaviours of diprotic acid-containing hydrogels. J Polym Sci 40:2969–2974Google Scholar
  16. 16.
    Uzun C, Hassnisaber M, Şen M, Güven O (2003) Enhancement and control of crosslinking of dimethylaminoethyl methacrylate irradiated at low dose rate in the presence of ethylene glycol dimethacrylate. Nucl Inst Methods Phys Res B 208:242–246CrossRefGoogle Scholar
  17. 17.
    De Paula R, Rodrigues J (1995) Composition and rheological properties of cashew tree gum, the exudate polysaccharide from Anacardium occidentale L. Carb Polym 26:177CrossRefGoogle Scholar
  18. 18.
    Ferruzzi G, Pan N, Casey W (2000) Mechanical properties of gellan and polyacrylamide gels with implications for soil stabilization. Soil Sci 165:778CrossRefGoogle Scholar
  19. 19.
    Şen M, Aguş O, Safrany A (2007) Controlling of pore size and distribution of PDMAEMA hydrogels prepared by gamma rays. Radiat Phys Chem 76:1342–1346CrossRefGoogle Scholar
  20. 20.
    Treloar LRG (1975) The physics of rubber elasticity, 3rd edn. Clarendon, OxfordGoogle Scholar
  21. 21.
    Peppas NA, Mikos AG (1986) Preparation methods and structure of hydrogels in medicine and pharmacy. Hyd Med Pharm 1:27–54Google Scholar
  22. 22.
    Carr DA, Peppas NA (2009) Molecular structure of physiologically-responsive hydrogels controls diffusive behavior. Macromol Biosci 9:497–505CrossRefPubMedPubMedCentralGoogle Scholar
  23. 23.
    Zhao F, Zhao S, Weina BO, Kuhn W, Blieskastel YJ (2007) Characterization of elastomer networks by NMR parameters Part I sulfur-cured NR networks. KGK 60:554–558Google Scholar
  24. 24.
    Ammar Nour Elhouda Ben, Saied Taib, Mejri Arbi, Hosni Faouzi, Mnif Adel, Hamzaoui Ahmed Hichem (2016) Study of agar proportions effect on a gamma ray synthesized hydrogel. J Mater Sci Eng A 6:87–99Google Scholar
  25. 25.
    Abad LV, Relleve LS, Aranilla CT, Dela Rosa AM (2003) Properties of radiation synthesized PVP-kappa carrageenan hydrogel blends. Rad Phys Chem 68(5):901–908CrossRefGoogle Scholar
  26. 26.
    Fechine GJM, Barros JAG, Alcântara MR, Catalani LH (2006) Fluorescence polarization and rheological studies of the poly(N-vinyl-2-pyrrolidone) hydrogels produced by UV radiation. Polymer 47:2629–2633CrossRefGoogle Scholar
  27. 27.
    Dispenza C, Grimaldi N, Sabatino M, Todaro S, Bulone D, Giacomazza D (2012) Studies of network organization and dynamics of e-beam crosslinked PVPs: from macro to nano. Radiat Phys Chem 81:1349–1353CrossRefGoogle Scholar
  28. 28.
    Wang M, Xu L, Hu H, Zhai M, Peng J, Nho Y, Li J, Wei G (2007) Radiation synthesis of PVP/CMC hydrogels as wound dressing. Nucl Instr Methods Phys Res Sect B 265:385–389CrossRefGoogle Scholar
  29. 29.
    Fratricova M, Schwarzer P (2006) 1H-NMR relaxation study of crosslinking and aging processes in polyurethane coatings. KGK 59:229–235Google Scholar
  30. 30.
    Benamer S, Mahlous M, Boukrif A, Mansouri B, Youcef SL (2006) Synthesis and characterisation of hydrogels based on poly(vinyl pyrrolidone). Nucl Instr Methods Phys Res Sect B 248:284–290CrossRefGoogle Scholar
  31. 31.
    Makuuchi K (2010) Critical review of radiation processing of hydrogel and polysaccharide. Radiat Phys Chem 79:267–271CrossRefGoogle Scholar
  32. 32.
    Bardajee GR, Pourjavadia A, Sheikh N, Amini-Fazl MS (2008) Grafting of acrylamide onto kappa-carrageenan via gamma-irradiation: optimization and swelling behavior. Radiat Phys Chem 77:131–137CrossRefGoogle Scholar
  33. 33.
    An J, Weaver A, Kim B, Barkatt A, Poster D, Vreeland WN, Silverman J, Al-sheikhly M (2011) Radiation-induced synthesis of poly (vinylpyrrolidone) nanogel. Polymer 52:5746–5755CrossRefGoogle Scholar
  34. 34.
    Demeter M, Virgolici M, Vancea C, Scarisoreanu A, Georgiana M, Kaya A, Meltzer V (2017) Network structure studies on γ–irradiated collagen–PVP superabsorbent hydrogels. Radiat Phys Chem 131:51–59CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2017

Authors and Affiliations

  • Nour Elhouda Ben Ammar
    • 1
    Email author
  • Taib Saied
    • 2
  • Mohamed Barbouche
    • 3
  • Faouzi Hosni
    • 4
  • Ahmed Hichem Hamzaoui
    • 1
  • Murat Şen
    • 5
  1. 1.Laboratory of Useful Materials Valuation, National Center for Research in Materials SciencesBorj Cedria TechnoparkSolimanTunisia
  2. 2.Laboratory of Analytical Chemistry and Electrochemistry, Sciences Faculty of TunisUniversity of Tunis El-ManarTunisTunisia
  3. 3.Laboratory of Nanomaterials and Systems for Renewable Energy, Research and Technologies Centre of EnergyTechnopark of Borj-CedriaHammamlifTunisia
  4. 4.Treatment Unit by Ionizing RadiationNational Center of Sciences and Nuclear Technology, Sidi Thabet TechnoparkSidi ThabetTunisia
  5. 5.Polymer Chemistry Division, Department of ChemistryHacettepe UniversityBeytepe AnkaraTurkey

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