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Toward Unimolecular Micelles with Tunable Dimensions Using Hyperbranched Dendritic-Linear Polymers
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.ORCID iD: 0000-0001-9035-4547
KTH, School of Biotechnology (BIO), Glycoscience. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.ORCID iD: 0000-0003-3572-7798
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2014 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 15, no 6, 2235-2245 p.Article in journal (Refereed) Published
Abstract [en]

A library of amphiphilic, hyperbranched dendritic-linear polymers (HBDLPs) are successfully synthesized, and evaluated as potential unimolecular micelles. Hyperbranched macroinitiators (HBMI), extended with poly(ethylene glycol) methacrylate (P(OEGMA)), are afforded via a combination of self-condensing vinyl (co)polymerization (SCV(C)P) and atom transfer radical polymerization (ATRP), providing a versatile two-step synthetic route. The HBDLP architecture and chain lengths are varied, and the effect on the nanoparticle (NP) stability and properties are evaluated. The HBDLPs form predominantly stable and spherical NPs, and the NP dimensions could be tailored by the HBDLP characteristics. The NPs formed are of high molecular weight, and their stability varies with the properties of the corresponding HBDLP. Too small dendritic segment, or too low degree of PEGylation, results to some extent in NP aggregation, while higher molecular weight HBDLPs, with a high amount of hydrophilic segments, appears to form discrete unimolecular micelles. The versatility of the platform is further demonstrated by the convenience of forming a HBDLP. with a more complex, linear copolymer extension instead of P(OEGMA).

Place, publisher, year, edition, pages
2014. Vol. 15, no 6, 2235-2245 p.
Keyword [en]
Condensing Vinyl Polymerization, Living Radical Polymerization, Block-Copolymer Hybrids, AB-Asterisk Monomers, Breast-Cancer Cells, In-Vitro Evaluation, Drug-Delivery, Biological Applications, Star Polymers, Nanoparticles
National Category
Other Chemistry Topics
URN: urn:nbn:se:kth:diva-148228DOI: 10.1021/bm5003637ISI: 000337497100031ScopusID: 2-s2.0-84902158485OAI: diva2:736106
Swedish Research Council, 2011-3720 2009-3259

QC 20140805

Available from: 2014-08-05 Created: 2014-08-04 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.
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:32
National Category
Polymer Technologies
Research subject
Chemical Engineering
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)
Swedish Research Council

QC 20150909

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

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