Colloid and Polymer Science

, Volume 297, Issue 9, pp 1233–1243 | Cite as

The influences of poly (ethylene glycol) chain length on hydrophilicity, oxygen permeability, and mechanical properties of multicomponent silicone hydrogels

  • Xueqin ZhangEmail author
  • Lu Wang
  • Huiwen Tao
  • Ying Sun
  • Hong Yang
  • Baoping LinEmail author
Original Contribution


Two series of multicomponent silicone hydrogels based on poly (ethylene glycol)- polydimethylsiloxane-poly (ethylene glycol) (PEG-PDMS-PEG) triblock oligomers were prepared by copolymerization of silicon-containing monomers methacrylate-terminated PEG-PDMS-PEG (MTSM), tris (trimethylsiloxy)-3-methacryloxpropylsilane (TRIS), and hydrophilic monomers such as N,N-dimethylacrylamide (DMA), N-vinylpyrrolidone (NVP), and hydroxypropyl-methacrylate (HPMA). The influences of PEG chain length on hydrophilicity, oxygen permeability, and mechanical properties of silicone hydrogels were explored. The hydrophilic properties of silicone hydrogels were characterized by water contact angle, equilibrium water content, and swelling-dehydration process. The results showed that the water contact angles of dry samples decreased while the swollen ones increased with the increase of PEG chain length. The equilibrium water content decreased first and then increased as the length of the PEG chain increased. The results of swelling and dehydration process showed that PEG chains improved the water-retaining capacity of silicone hydrogels. Moreover, the protein adsorption of samples with PEG chains decreased. The surface morphologies of silicone hydrogels were characterized by scanning electron microscope (SEM), and a reconstruction model was proposed. In addition, the oxygen permeability and mechanical properties of silicone hydrogels also varied with the length of the PEG chain. These results could provide a theoretical reference for the design and modification of new hydrogels.

Graphical abstract

The properties of silicone hydrogels obtained by copolymerization of MTSM with hydrophilic monomers vary with the chain length of PEG, when PEG chains are presented as a segment of MTSM.


Silicone hydrogels PEG chains Hydrophilicity Oxygen permeability Mechanical properties 


Funding information

This work was financially supported by the Natural Science Foundation of Jiangsu Province (BK20130617, BK20130619), the National Natural Science Foundation of China (Grant No. 21374016, 21304018), and the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflicts of interest.

Supplementary material

396_2019_4544_MOESM1_ESM.docx (606 kb)
ESM 1 (DOCX 605 kb)


  1. 1.
    Tighe BJ (2013) A decade of silicone hydrogel development: surface properties, mechanical properties, and ocular compatibility. Eye Contact Lens 39(1):4–12Google Scholar
  2. 2.
    Sugimoto H, Nishino G, Tsuzuki N, Daimatsu K, Inomata K, Nakanishi E (2012) Preparation of high oxygen permeable transparent hybrid copolymers with silicone macro-monomers. Colloid Polym Sci 290(2):173–181Google Scholar
  3. 3.
    Nicolson PC, Vogt J (2001) Soft contact lens polymers: an evolution. Biomaterials 22(24):3273–3283Google Scholar
  4. 4.
    Caló E, Khutoryanskiy VV, Reading TUo (2015) Biomedical applications of hydrogels: a review of patents and commercial products. Eur Polym J 65:252–267Google Scholar
  5. 5.
    Morales-Hurtado M, Zeng X, Gonzalez-Rodriguez P, Elshof JET, Heide EVD (2015) A new water absorbable mechanical epidermal skin equivalent: the combination of hydrophobic PDMS and hydrophilic PVA hydrogel. J Mech Behav Biomed Mater 46:305–317Google Scholar
  6. 6.
    Hamid ZAA, Lim KW (2016) Evaluation of UV-crosslinked poly (ethylene glycol) diacrylate/poly (dimethylsiloxane) dimethacrylate hydrogel: properties for tissue engineering application. Proc Chem 19:410–418Google Scholar
  7. 7.
    Xu J, Li X, Sun F (2011) In vitro and in vivo evaluation of ketotifen fumarate-loaded silicone hydrogel contact lenses for ocular drug delivery. Drug Deliv 18(2):150–158Google Scholar
  8. 8.
    Wang J, Fang L, Wei J (2012) Hydrophilic silicone hydrogels with interpenetrating network structure for extended delivery of ophthalmic drugs. Polym Adv Technol 23(9):1258–1263Google Scholar
  9. 9.
    Rudy A, Kuliasha C, Uruena J, Rex J, Schulze KD, Stewart D, Angelini T, Sawyer WG, Perry SS (2017) Lubricous hydrogel surface coatings on polydimethylsiloxane (PDMS). Tribol Lett 65(1):3Google Scholar
  10. 10.
    Oláh A, Hillborg H, Vancso GJ (2005) Hydrophobic recovery of UV/ozone treated poly (dimethylsiloxane): adhesion studies by contact mechanics and mechanism of surface modification. Appl Surf Sci 239(3):410–423Google Scholar
  11. 11.
    David T, Puccinelli JP, Beebe DJ (2006) Thermal aging and reduced hydrophobic recovery of polydimethylsiloxane. Sensors Actuators B Chem 114(1):170–172Google Scholar
  12. 12.
    Vlachopoulou ME, Petrou PS, Kakabakos SE, Tserepi A, Beltsios K, Gogolides E (2009) Effect of surface nanostructuring of PDMS on wetting properties, hydrophobic recovery and protein adsorption. Microelectron Eng 86(4):1321–1324Google Scholar
  13. 13.
    Bhattacharya S, Datta A, Berg JM, Gangopadhyay S (2005) Studies on surface wettability of poly (dimethyl) siloxane (PDMS) and glass under oxygen-plasma treatment and correlation with bond strength. J Microelectromech Syst 14(3):590–597Google Scholar
  14. 14.
    Kun M, Javier R, Hirasaki GJ, Sibani Lisa B (2011) Wettability control and patterning of PDMS using UV-ozone and water immersion. J Colloid Interface Sci 363(1):371–378Google Scholar
  15. 15.
    Yilgor E, Kaymakci O, Isik M, Bilgin S, Yilgor I (2012) Effect of UV/ozone irradiation on the surface properties of electrospun webs and films prepared from polydimethylsiloxane–urea copolymers. Appl Surf Sci 258(10):4246–4253Google Scholar
  16. 16.
    Charles W, Schmidt G, Wilker JJ (2013) A review on tough and sticky hydrogels. Colloid Polym Sci 291(9):2031–2047Google Scholar
  17. 17.
    Tang Q, Yu JR, Chen L, Zhu J, Hu ZM (2011) Poly (dimethyl siloxane)/poly (2-hydroxyethyl methacrylate) interpenetrating polymer network beads as potential capsules for biomedical use. Curr Appl Phys 11(3):945–950Google Scholar
  18. 18.
    Mark VB, Andrea W, Lyndon J, Heather S (2008) Immobilized hyaluronic acid containing model silicone hydrogels reduce protein adsorption. J Biomater Sci Polym Ed 19(11):1425–1436Google Scholar
  19. 19.
    Lin G, Zhang X, Kumar SR, Mark JE (2010) Modification of polysiloxane networks for biocompatibility. Mol Cryst Liq Cryst 521(1):56–71Google Scholar
  20. 20.
    Yao M, Ji F (2012) Hydrophilic PEO-PDMS for microfluidic applications. J Micromech Microeng 22(2):025012Google Scholar
  21. 21.
    Garay RP, Raafat EG, Armstrong JK, George G, Pascal R (2012) Antibodies against polyethylene glycol in healthy subjects and in patients treated with PEG-conjugated agents. Exp Opin Drug Deliv 9(11):1319–1323Google Scholar
  22. 22.
    Demming S, Lesche C, Schmolke H, Klages CP, Büttgenbach S (2011) Characterization of long-term stability of hydrophilized PEG-grafted PDMS within different media for biotechnological and pharmaceutical applications. Phys Status Solidi 208(6):1301–1307Google Scholar
  23. 23.
    Vladkova T (2010) Surface modification of silicone rubber with poly (ethylene glycol) hydrogel coatings. J Appl Polym Sci 92(3):1486–1492Google Scholar
  24. 24.
    Cui J, Lackey MA, Tew GN, Crosby AJ (2012) Mechanical properties of end-linked PEG/PDMS hydrogels. Macromolecules 45(15):6104–6110Google Scholar
  25. 25.
    Rutnakornpituk M, Ngamdee P, Phinyocheep P (2006) Preparation and properties of polydimethylsiloxane-modified chitosan. Carbohydr Polym 63(2):229–237Google Scholar
  26. 26.
    Fatona A, Chen Y, Reid M, Brook MA, Moran-Mirabal JM (2015) One-step in-mould modification of PDMS surfaces and its application in the fabrication of self-driven microfluidic channels. Lab Chip 15(22):4322–4330. Google Scholar
  27. 27.
    Peng S, Guo Q, Hughes TC, Hartley PG (2011) In SituSynchrotron SAXS study of Polymerizable microemulsions. Macromolecules 44(8):3007–3015. Google Scholar
  28. 28.
    Tao H, Zhang X, Sun Y, Yang H, Lin B (2016) The influence of molecular weight of siloxane macromere on phase separation morphology, oxygen permeability, and mechanical properties in multicomponent silicone hydrogels. Colloid Polym Sci 295(1):205–213. Google Scholar
  29. 29.
    Maldonado-Codina C, Morgan PB (2007) In vitro water wettability of silicone hydrogel contact lenses determined using the sessile drop and captive bubble techniques. J Biomed Mater Res A 83(2):496–502. Google Scholar
  30. 30.
    Maghsoudy-Louyeh S, Ju HS (2010) Tittmann BR surface roughness study in relation with hydrophilicity/hydrophobicity of materials using atomic force microscopyGoogle Scholar
  31. 31.
    Shirtcliffe NJ, Mchale G, Atherton S, Newton MI (2010) An introduction to superhydrophobicity. Adv Colloid Interf Sci 161(1):124–138Google Scholar
  32. 32.
    Sundaram HS, Cho Y, Dimitriou MD, Weinman CJ, Finlay JA, Cone G, Callow ME, Callow JA, Kramer EJ, Ober CK (2011) Fluorine-free mixed amphiphilic polymers based on PDMS and PEG side chains for fouling release applications. Biofouling 27(6):589–602. Google Scholar
  33. 33.
    Zhang Y, Lin Y (2011) Improvement of permeability of poly (vinyl alcohol) hydrogel by using poly (ethylene glycol) as Porogen. J Macromol Sci D Rev Polym Process 50(8):776–782Google Scholar
  34. 34.
    Xiaole MA, Yanlei SU, Qiang S, Wang Y, Jiang Z (2007) Preparation of protein-adsorption-resistant polyethersulfone ultrafiltration membranes through surface segregation of amphiphilic comb copolymer. J Membr Sci 292(1):116–124Google Scholar
  35. 35.
    Olanya G, Thormann E, Varga I, Makuska R, Claesson PM (2010) Protein interactions with bottle-brush polymer layers: effect of side chain and charge density ratio probed by QCM-D and AFM. J Colloid Interface Sci 349(1):265–274. Google Scholar
  36. 36.
    Latour RA (2005) Biomaterials: protein–surface interactionsGoogle Scholar
  37. 37.
    Berean K, Ou JZ, Nour M, Latham K, McSweeney C, Paull D, Halim A, Kentish S, Doherty CM, Hill AJ, Kalantar-zadeh K (2014) The effect of crosslinking temperature on the permeability of PDMS membranes: evidence of extraordinary CO2 and CH4 gas permeation. Sep Purif Technol 122:96–104. Google Scholar
  38. 38.
    Zhao Z, Xie H, An S, Jiang Y (2014) The relationship between oxygen permeability and phase separation morphology of the multicomponent silicone hydrogels. J Phys Chem B 118(50):14640–14647. Google Scholar
  39. 39.
    Sun G, Zhang XZ, Chu CC (2008) Effect of the molecular weight of polyethylene glycol (PEG) on the properties of chitosan-PEG-poly(N-isopropylacrylamide) hydrogels. J Mater Sci Mater Med 19(8):2865–2872. Google Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.School of Chemistry and Chemical EngineeringSoutheast UniversityNanjingPeople’s Republic of China

Personalised recommendations