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Polyester hydrogels with swelling properties controlled by the polymer architecture, molecular weight, and crosslinking agent
KTH, Superseded Departments, Polymer Technology.ORCID iD: 0000-0002-1922-128X
KTH, Superseded Departments, Polymer Technology.
2003 (English)In: Journal of Polymer Science Part A: Polymer Chemistry, ISSN 0887-624X, E-ISSN 1099-0518, Vol. 41, no 9, 1296-1305 p.Article in journal (Refereed) Published
Abstract [en]

Hydrogels of poly(1,5-dioxepan-2-one) and hydrogels of block copolymers of poly(1,5-dioxepan-2-one) and poly(L-lactide) were synthesized. Both star-shaped polymers and linear polymers were polymerized with ring-opening polymerization and crosslinked in situ with a tetrafunctional acid chloride (1,2,3,4-cyclopentane tetracarboxylic acid chloride) or a difunctional acid chloride (succinyl chloride). Different network architectures were synthesized in this way. The initial monomer concentrations and the molecular weights of the macromonomers were also altered. The networks were characterized with H-1 NMR and differential scanning calorimetry, and the swelling abilities of the different hydrogels were investigated in water and dichloromethane. The ratio of the monomer to the crosslinking agent was assessed by the quantification of the signal intensities in the H-1 NMR spectra of the swelled network and agreed with the theoretical crosslinking density. Both the homopolymers of 1,5-dioxepan-2-one and the copolymers of 1,5-dioxepan-2-one and L-lactide swelled to a high degree in water. The swelling properties of the materials could be varied over a broad range by changes in the architecture, molecular weight, and content of the precursor in the network. Star-shaped poly(1,5-dioxepan-2-one) crosslinked with a difunctional acid chloride had the highest degree of swelling among the different homopolymer hydrogels. This network also had the lowest glass-transition temperature because of the flexible units in the structure. The same trends found for the homopolymer hydrogels were also seen in the hydrogels with block copolymers. The hydrogels swelled enormously in dichloromethane, and as in water, the star-shaped copolymer crosslinked with a difunctional acid chloride had the highest degree of swelling.

Place, publisher, year, edition, pages
2003. Vol. 41, no 9, 1296-1305 p.
Keyword [en]
hydrogels, architecture, polyesters, crosslinking, swelling, RING-EXPANSION POLYMERIZATION, POLY(ETHYLENE GLYCOL), EPSILON-CAPROLACTONE, L-LACTIDE, MACROCYCLIC POLYMERIZATION, BIODEGRADABLE NETWORKS, OPENING POLYMERIZATION, POLYLACTONES, 1, 5-DIOXEPAN-2-ONE, INITIATORS
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-13189DOI: 10.1002/pola.10682ISI: 000182114700012OAI: oai:DiVA.org:kth-13189DiVA: diva2:321697
Note
QC 20100602Available from: 2010-06-02 Created: 2010-06-02 Last updated: 2017-12-12Bibliographically approved
In thesis
1. Novel Possibilities for Advanced Molecular Structure Design for Polymers and Networks
Open this publication in new window or tab >>Novel Possibilities for Advanced Molecular Structure Design for Polymers and Networks
2003 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

Synthetic and degradable polymers are an attractive choicein many areas, since it is possible to control the way in whichthey are manufactured; more specifically, pathways tomanipulate the architecture, the mechanical properties and thedegradation times have been identified. In this work,L-lactide, 1,5-dioxepan-2-one and ε-caprolactone were usedas monomers to synthesize polymers with different architecturesby ring-opening polymerization. By using novel initiators,triblock copolymers, functionalized linear macromonomers andstar-shaped aliphatic polyesters with well-defined structureshave been synthesized. To synthesize triblock copolymers,cyclic germanium initiators were studied. The polymerizationproceeded in a controlled manner although the reaction rateswere low. To introduce functionality into the polymer backbone,functionalized cyclic tin alkoxides were prepared and used asinitiators. During the insertion-coordination polymerization,the initiator fragment consisting mainly of a double bond wasincorporated into the polymer backbone. The double bond wasalso successfully epoxidized and this gave unique possibilitiesof synthesizing graft polymers with precise spacing. Themacromonomer technique is a very effective method for producingwell-defined graft polymers. Spirocyclic tin initiators weresynthesized and used to construct star-shaped polymers. Thestar-shaped polymers were subsequently crosslinked in apolycondensation reaction. These crosslinked structures swelledin water, and swelling tests showed that by changing thestructure of the hydrogel network, the degree of swelling canbe altered. A first evaluation of the surface characteristicsof the linear triblock copolymers was also performed. AFManalysis of the heat-treated surfaces revealed nanometer-scalefibers and tests showed that keratinocytes were able to growand proliferate on these surfaces.

Place, publisher, year, edition, pages
Stockholm: KTH, 2003. 78 p.
Keyword
ring-opening polymerization, coordination-insertion, germanium, cyclic tin alkoxides, spirocyclic initiators, poly(L-lactide), poly(1, 5-dioxepan-2-one), triblock, star-shaped, network, functionalization, morphology, AFM
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-3623 (URN)91-7283-577-X (ISBN)
Public defence
2003-10-31, 00:00 (English)
Note
QC 20100602Available from: 2003-10-28 Created: 2003-10-28 Last updated: 2010-06-02Bibliographically approved

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