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Sequential interpenetrating poly(ethylene glycol) hydrogels prepared by UV-initiated thiol–ene coupling chemistry
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.ORCID iD: 0000-0002-9200-8004
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.ORCID iD: 0000-0002-9372-0829
2013 (English)In: Journal of Polymer Science Part A: Polymer Chemistry, ISSN 0887-624X, E-ISSN 1099-0518, Vol. 51, no 2, 363-371 p.Article in journal (Refereed) Published
Abstract [en]

Poly(ethylene glycol) (PEG)-diallyls, ranging from 2 to 8 kDa, were successfully reacted with a trifunctional thiol crosslinker via thiol–ene coupling reaction to construct four different primary PEG hydrogels. These systems were used as scaffolds for the preparation of a library of sequential interpenetrating networks (SeqIPNs). The solid content of the secondary networks varied between 21 and 34% and was dependent on the length of the absorbing PEGs. The gel fractions for the IPNs were above 85%. Additionally, the lowest degree of swelling was found for the IPN based on 2-kDa PEG (315%), whereas the 8-kDa PEG IPN exhibited a value of 810%. The SeqIPN strategy facilitated hydrogel systems that cover a larger domain of tensile modulus (192–889 kPa) when compared with single hydrogel networks (175–555 kPa).

Place, publisher, year, edition, pages
2013. Vol. 51, no 2, 363-371 p.
Keyword [en]
hydrogels, modulus, networks, polyethers, poly(ethylene glycol), swelling degree, thiol–ene click chemistry, UV curing
National Category
Polymer Technologies
Identifiers
URN: urn:nbn:se:kth:diva-105557DOI: 10.1002/pola.26393ISI: 000312448800016Scopus ID: 2-s2.0-84870981886OAI: oai:DiVA.org:kth-105557DiVA: diva2:571463
Funder
Swedish Research Council, 2010-453
Note

QC 20121122

Available from: 2012-11-22 Created: 2012-11-22 Last updated: 2017-12-07Bibliographically approved
In thesis
1. Mechanical and swelling properties of hydrogels
Open this publication in new window or tab >>Mechanical and swelling properties of hydrogels
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Hydrogels have been used as one of the novel soft materials in many biomedical applications such as drug delivery and tissue engineering for recent decades.

In the main part of this work, bi-functional poly(ethylene glycol) (PEG) precursors with either thiols (PEG-SH) or allyls (PEG-Al) , covering molecular weights from 3 kDa to 8 kDa were synthesized and thoroughly characterized by 1H NMR, 13C NMR, FT-Raman and MALDI-TOF techniques. By combining PEG precursors with complementary trifunctional crosslinkers, a library of well-defined single-network hydrogels was efficiently constructed via the robust UV-initiated thiol-ene coupling (TEC) chemistry. Novel sequential interpenetrating network (seqIPN) hydrogels based on PEG were fabricated by diffusing and afterwards crosslinking secondary-network precursors within dense (2 kDa) to loose (8 kDa) primary networks. The impacts of polymer chain length and diffusion time on the swelling and mechanical properties were assessed for the seqIPN hydrogels. Additionally, disperse red 13 decorated PEG 2 kDa and 8 kDa were synthesized and used as probes to monitor the secondary-network precursor diffusion rate by UV/Vis spectroscopy. 

FT-Raman and leaching tests were conducted to evaluate the efficiency of the TEC reaction for the development of PEG networks and their gel fractions. All gels were fully crosslinked within 5 minutes and with the gel fraction above 84%. The chain length of PEG, location of functional groups of PEGs, solvents, solid content were found to have directly influence on the mechanical and swelling properties of PEG single-network hydrogels. The utilization of the diffusion time dependent seqIPN strategy enabled further freedom to control the swelling and mechanical properties of PEG hydrogels, with the degree of water swelling ranged from 280 – 870% and the tensile modulus ranging from 1135 kPa to 175 kPa.

Furthermore, the seqIPN strategy was utilized for fiber reinforced free radical polymerized hydrogels. N, N-dimethylacrylamide (DMA) with crosslinker poly(ethylene glycol) diacrylate were diffused in bacterial cellulose (BC) aerogel thereafter UV crosslinked to form BC-DMA hydrogels. FT-Raman and leaching tests were conducted to evaluate the efficiency of the free radical polymerization and the BC-DMA gel fractions. After UV cure for 10 minutes, robust DMA networks were formed within BC aerogels with over 94% gel fraction. The high porosity and robust interpenetrating DMA network within BC fibers were further analysed with FE-SEM. Compression tests showed that fiber reinforced DMA hydrogels have higher compression modulus than DMA hydrogels, ranging from 4.4 to 8.3 MPa with water content from 78 to 70%.

Place, publisher, year, edition, pages
KTH: KTH Royal Institute of Technology, 2012. 67 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2012:63
National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-105539 (URN)978-91-7501-471-5 (ISBN)
Public defence
2012-12-06, F3, Lindstedtsvägen 26, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 2012

Available from: 2012-11-22 Created: 2012-11-22 Last updated: 2012-11-22Bibliographically approved

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Malkoch, MichaelHult, Anders

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