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Thermo-responsive cellulose-based architectures: tailoring LCST using poly(ethylene glycol) methacrylates
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.ORCID iD: 0000-0001-9035-4547
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.ORCID iD: 0000-0002-8348-2273
2011 (English)In: POLYMER CHEMISTRY, ISSN 1759-9954, Vol. 2, no 5, 1114-1123 p.Article in journal (Refereed) Published
Abstract [en]

There is a growing interest in designing advanced macromolecular architectures applicable for instance in drug delivery systems. Employing cellulose in these systems is particularly favorable due to attractive properties such as biocompatibility and low price. Additionally, thermo-responsive polymers of poly(ethylene glycol) methacrylates are promising in this field owing to their biocompatibility and non-toxicity. In the present study, amphiphilic thermo-responsive homo- and copolymers of oligo(ethylene glycol) methyl ether methacrylate (OEGMA(300)) and di(ethylene glycol) methyl ether methacrylate (DEGMA) were synthesized via ARGET ATRP. Both linear copolymers of DEGMA/OEGMA(300) as well as comb architectures with copolymers of DEGMA/OEGMA(300) grafted from hydroxypropyl cellulose were produced. The lower critical solution temperature of the linear copolymers was readily tailored by altering the monomer feed ratio. The grafting of the thermo-responsive polymers from hydroxypropyl cellulose resulted in a consistent decrease of the lower critical solution temperature compared to the linear analogues; however, interestingly the ability to tune the transition temperature remained. Moreover, the amphiphilic comb architectures formed polymeric micelles with low critical micelle concentrations. Consequently, these advanced architectures combine the favorable properties of hydroxypropyl cellulose with the interesting thermo-responsive and stealth properties of poly(ethylene glycol) methacrylates, and may, therefore, find potential applications in biomedicine.

Place, publisher, year, edition, pages
2011. Vol. 2, no 5, 1114-1123 p.
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-34355DOI: 10.1039/c0py00417kISI: 000290681800015Scopus ID: 2-s2.0-79955864168OAI: oai:DiVA.org:kth-34355DiVA: diva2:435312
Funder
Swedish Research Council
Note
QC 20110818Available from: 2011-08-18 Created: 2011-06-07 Last updated: 2015-09-09Bibliographically approved
In thesis
1. Exploring Amphiphilic PEGMA-Based Architectures as Nanoparticles for Drug Delivery
Open this publication in new window or tab >>Exploring Amphiphilic PEGMA-Based Architectures as Nanoparticles for Drug Delivery
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Within the last decades, the stated potential of polymer constructs as drug delivery systems have challenged researchers to develop sophisticated polymers with tunable properties. The versatility of polymers makes them highly attractive to tailor nanoparticles (NPs) which fulfill the demands of effective drug delivery systems (DDS). The aim of this work was to design and synthesize amphiphilic ethylene glycol methacrylate-based (EGMA) macromolecules, and explore their potential as NPs for drug delivery.

Initially, a study of the controlled synthesis and solution properties of linear EGMA polymers, as well as the potential to transfer their behavior to amphiphilic comb copolymers, was conducted. Well-controlled polymers with interesting tunable thermo-responsive properties were accomplished by altering the monomer feed ratio. Furthermore, the comb copolymers formed self-assembled core-shell type structures in aqueous solution.

A library of amphiphilic fluorinated polymers was successfully established to explore the potential of EGMA-based polymers in a dual-functional theranostic delivery system. The non-toxic polymers self-assembled into small “stealthy” NPs, and the combination of fluorinated segments with EGMA segments allowed for detection by 19F-MRI with good imaging properties. The hydrophobic core of the NPs was capable to encapsulate and release an anti-cancer therapeutic, and effectively reduced the viability of three different cancer cell lines. The diffusion-controlled release kinetics of the drug from the NPs interestingly depended on the nature of the core moiety.

To reduce issues with instability of self-assembling NP systems the possibility to synthesize amphiphilic hyperbranched dendritic-linear polymers (HBDLPs) was investigated. Their three-dimensional structure was hypothesized to facilitate stabilization as unimolecular micelles. The architecture, hydrophilic/hydrophobic ratio, and high molecular weight showed to be crucial to avoid polymer association and stabilize the HBDLPs individually. In addition, the hyperbranched core of the HBDLPs was readily functionalized with disulfide bonds, either in the backbone or in the pendant groups. Under reductive conditions, selective cleavage of the disulfides thereby enabled either significant molecular weight reduction, or allowed for triggered release of a covalently bound dye, mimicking a drug. Potentially, such HBDLPs could be stable during circulation, while allowing for selective degradation and/or therapeutic release upon delivery to a cancer tissue.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. 69 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:32
National Category
Polymer Technologies
Research subject
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-173242 (URN)978-91-7595-630-5 (ISBN)
Public defence
2015-10-02, F3, Lindstedtsvägen 26, KTH, Stockholm, 09:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council
Note

QC 20150909

Available from: 2015-09-09 Created: 2015-09-08 Last updated: 2015-09-09Bibliographically approved

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Porsch, ChristianMalmström Jonsson, Eva

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