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Phase Phenomena in Polymer Networks: Empirical Studies on the Influence of Hydrophobicity, Charge Density and Crosslinks on Macroion-Induced Phase Transitions in Polyelectrolyte Gels
Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy. (Farmaceutisk Fysikalisk Kemi)
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The thesis concerns polyelectrolyte gels in contact with oppositely charged proteins and surfactant micelles, and includes of four papers (I-IV). In paper I confocal Raman spectroscopy was introduced as a method to trace micelles and investigate the structure of gel-surfactant complexes, in phase separated gel spheres. In paper II, the binding of surfactants to microspheres (~50-100 µm) was investigated by means of a micromanipulator-assisted microscopy method. The two surfactants were found to display qualitative difference respect to degree of swelling, surfactant distribution in the gels, and the difference is discussed in terms of absence/presence of hydrophobic attraction to the polyelectrolyte gel network. Kinetics of volume change in gels were analyzed. Aggregation numbers of micelles in polystyrenesulfonate (PSS) solutions, obtained from fluorescence quenching measurements, are presented. In paper III, phase behaviour, protein assembly and diffusion, was studied in PSS gel microspheres. Interpretation of results was aided by measurements of osmotic swelling of individual gel networks, and by combining the results with studies of protein diffusion in macroscopic (cm-sized) gel spheres. Complexes formed were further analyzed with small angle x-ray spectroscopy. In paper IV phase behaviour of mixed ionic/nonionic surfactant micelles is investigated in cm-sized gel spheres. The coexistence of three phases, the formation of dense shells in the bulk of the gels and other phenomena are described for the first time, and the results are presented along with discussion on the charge-density of spherical micelles and of  network induced hysteresis effects in gels. The composition and microstructure of phases are investigated by confocal Raman spectroscopy and small-angle x-ray scattering respectively. The results are interpreted with aid of highly detailed theoretical model calculations.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis , 2011. , p. 53
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Pharmacy, ISSN 1651-6192 ; 137
Keyword [en]
Gel, microgel, microsphere, polystyrenesulfonate, polyacrylate, polyacrylicacid, DoTAB, DoTAC, CTAB, CTAC, network, polyelectrolyte, complex salt, self assembly, phase behaviour, hysteresis, thermodynamic, core-shell, lysozyme, cytochrome c, microscopy, micromanipulator, elastomer, elastic, protein, surfactant, phase behaviour, sorting
National Category
Pharmaceutical Sciences Physical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-145381ISBN: 978-91-554-8001-1 (print)OAI: oai:DiVA.org:uu-145381DiVA, id: diva2:396048
Public defence
2011-03-18, B42, BMC, Husargatan 3, Uppsala, 12:30 (Swedish)
Opponent
Supervisors
Available from: 2011-02-24 Created: 2011-02-08 Last updated: 2018-01-12
List of papers
1. Differences in binding of a cationic surfactant to cross-linked sodium poly(acrylate) and sodium poly(styrene sulfonate) studied by Raman spectroscopy
Open this publication in new window or tab >>Differences in binding of a cationic surfactant to cross-linked sodium poly(acrylate) and sodium poly(styrene sulfonate) studied by Raman spectroscopy
2005 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 21, no 7, p. 2761-2765Article in journal (Refereed) Published
Abstract [en]

Raman spectroscopy has been used to investigate the structure of gel-surfactant complexes. Cross-linked sodium poly(acrylate) and sodium poly(styrene sulfonate) were immersed in solutions of the cationic surfactant dodecyl trimethylammonium bromide. During the deswelling process, two distinct regions could be observed for both types of gels. Looking at the Raman spectra, however, for the poly(styrene sulfonate), the surfactant could be found throughout the gel particle, whereas for poly(acrylate), essentially all the surfactant was bound in a surface layer.

National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-70227 (URN)10.1021/la0468693 (DOI)15779946 (PubMedID)
Available from: 2008-12-16 Created: 2008-12-16 Last updated: 2017-11-21
2. Single microgel particle studies demonstrate the influence of hydrophobic interactions between charged micelles and oppositely charged polyions.
Open this publication in new window or tab >>Single microgel particle studies demonstrate the influence of hydrophobic interactions between charged micelles and oppositely charged polyions.
2005 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 21, no 9, p. 3773-3781Article in journal (Refereed) Published
Abstract [en]

The binding of two cationic surfactants, dodecyltrimethylammonium bromide (DoTAB) and N-(1,1,2,2-tetrahydroperfluorodecanyl)pyridinium bromide (HFDePB), to covalently cross-linked sodium poly(styrenesulfonate) (PSS) microgels has been investigated by means of micromanipulator-assisted time-resolved light microscopy on single gels. It is demonstrated that repeated measurements on the same microgel under conditions of controlled liquid flow give highly reproducible results. The two surfactants are found to behave very differently with respect to degree of swelling, surfactant distribution in the gels, both during shrinking and at equilibrium, and kinetics of volume changes induced by them. The main difference is attributed to the presence of a hydrophobic interaction between PSS and the DoTAB micelles, absent in the case of HFDePB. Kinetic shrinking curves are recorded and analyzed using a model for steady-state transport of surfactant between the solution and the gels. Aggregation numbers for DoTAB in PSS solutions obtained from fluorescence quenching measurements are presented. A strong dependence on the surfactant-to-polyion concentration ratio is observed. Relations between surfactant binding isotherms, phase diagrams for linear polyelectrolyte/surfactant/water systems, and the binding to gels are discussed.

National Category
Medical and Health Sciences
Identifiers
urn:nbn:se:uu:diva-92344 (URN)10.1021/la047316v (DOI)15835936 (PubMedID)
Available from: 2004-10-29 Created: 2004-10-29 Last updated: 2017-12-14Bibliographically approved
3. Lysozyme Incorporation in Poly(styrenesulfonate) Microspheres: Dynamics of Core/Shell formation
Open this publication in new window or tab >>Lysozyme Incorporation in Poly(styrenesulfonate) Microspheres: Dynamics of Core/Shell formation
(English)Manuscript (preprint) (Other academic)
Identifiers
urn:nbn:se:uu:diva-145378 (URN)
Available from: 2011-02-08 Created: 2011-02-08 Last updated: 2011-02-24
4. Mixed Micelles in Spherical Polyelectrolyte Networks: Influence of Crosslinks on Charge Induced Phase Separation
Open this publication in new window or tab >>Mixed Micelles in Spherical Polyelectrolyte Networks: Influence of Crosslinks on Charge Induced Phase Separation
(English)Manuscript (preprint) (Other academic)
Identifiers
urn:nbn:se:uu:diva-145379 (URN)
Available from: 2011-02-08 Created: 2011-02-08 Last updated: 2011-02-24

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