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Formation and Stability of Water-Soluble Molecular Polyelectrolyte Complexes: Effects of Charge Density, Mixing Ratio and Polyelectrolyte Concentration
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
YKI, Institute of Surface Chemistry.
Dept of Polymer Chemistry, Vilnius University, Lithania.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
2009 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 25, no 11, 6113-6121 p.Article in journal (Refereed) Published
Abstract [en]

The formation of complexes with stoichiometric (1:1) as well as nonstoichiometric (2:1) and (1:2) compositions between oppositely charged synthetic polyelectrolytes carrying strong ionic groups and significantly different molecular weights is reported in this contribution. Poly(sodium styrenesulfonate) (NaPSS) was used as polyanion, and a range of copolymers with various molar ratios of the poly(methacryloxyethyltrimethylammonium) chloride, poly(METAC), and the nonionic poly(ethylene oxide) ether methacrylate, poly(PEO45MEMA), were used as polycations. Formation and stability of PECs have been investigated by dynamic and static light scattering (LS), turbidity, and electrophoretic mobility measurements as a function of polyelectrolyte solution concentration, charge density of the cationic polyelectrolyte, and mixing ratio. The data obtained demonstrate that in the absence of PEO45 side chains the 100% charged polymer (polyMETAC) formed insoluble PECs with PSS that precipitate from solution when exact stoichiometry is achieved. In nonstoichiometric complexes (1:2) and (2:1) large colloidally stable aggregates were formed. The presence of even a relatively small amount of PEO45 side chains (25%) in the cationic copolymer was sufficient for preventing precipitation of the formed stoichiometric and nonstoichiometric complexes. These PEC’s are sterically stabilized by the PEO45 chains. By further increasing the PEO45 side-chain content (50 and 75%) of the cationic copolymer, small, water-soluble molecular complexes could be formed. The data suggest that PSS molecules and the charged backbone of the cationic brush form a compact core, and with sufficiently high PEO45 chain density (above 25%) molecular complexes are formed that are stable over prolonged times.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2009. Vol. 25, no 11, 6113-6121 p.
Keyword [en]
ENTRAPPING ENZYME MOLECULES; DILUTE AQUEOUS-SOLUTION; SALT CONCENTRATION; BLOCK-COPOLYMERS; CHAIN-LENGTH; MICELLES; DELIVERY; POLYCATIONS; SCATTERING; GLYCOL
National Category
Other Chemistry Topics
Identifiers
URN: urn:nbn:se:kth:diva-70251ISI: 000266604000020Scopus ID: 2-s2.0-66749184130OAI: oai:DiVA.org:kth-70251DiVA: diva2:486124
Note
QC 20120207Available from: 2012-02-07 Created: 2012-01-30 Last updated: 2017-12-08Bibliographically approved
In thesis
1. Polyelectrolyte complexes of bottle brush copolymers: Solution and adsorption properties
Open this publication in new window or tab >>Polyelectrolyte complexes of bottle brush copolymers: Solution and adsorption properties
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The aim of this thesis work was to systematically investigate the physico-chemical properties of polyelectrolyte complexes (PECs) formed by bottle brush and linear polyelectrolytes in solution and at solid / liquid interfaces. Electrostatic self-assembly of oppositely charged macromolecules in aqueous solution is a versatile strategy to construction of functional nanostructures with easily controlled properties. Bottle brush architecture, introduced into the PEC, generates a number of distinctive properties of the complexes, related to a broad range of application, such as colloidal stability and protein repellency to name a few. To utilize these materials in a wide range of applications e.g. drug delivery, the understanding of the effects of polymer architecture and solution parameters on the properties of bottle brush PECs is of paramount importance. This thesis constitutes a systematic investigation of PECs formed by a series of cationic bottle-brush polyelectrolytes and a series of anionic linear polyelectrolytes in aqueous solution. The focus of the first part of the thesis was primarily on formation and characterization of PECs in solution, whereas the adsorption properties and adsorption kinetics of bottle-brush polyelectrolytes and their complexes was investigated in the second part of the thesis work. In particular, effects of the side-chain density of the bottlebrush polyelectrolyte, concentration, mixing ratio and molecular weigh of the linearpolyelectrolyte on formation, solution properties, stability and adsorption of PECs were addressed.

The pronounced effect of the side-chain density of the bottle-brush polyelectrolyte on the properties of stoichiometric and nonstoichiometric PECs was demonstrated. Formation of PECs by bottle-brush copolymers with high density of side-chains results in small, watersoluble, molecular complexes having nonspherical shape, independent of concentration. Whereas formation of PEC-aggregates was revealed by bottle-brush polyelectrolytes with low side chain density, the level of aggregation in these complexes is controlled by polyelectrolyte concentration. The structure of the PECs formed with low molecular weight polyanions is consistent with the picture that several small linear polyelectrolyte molecules associate with the large bottle-brush. In contrast, when complexation occurs between polyanions of high molecular weigh and the bottle-brush polymers considerably larger PECs are formed, consistent with several bottle-brush polymers associating with one high molecular weight polyanion.

Place, publisher, year, edition, pages
Stockholm: KTH-Royal Institute of Technology, 2011. xiii, 62 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2011:37
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-33666 (URN)978-91-7415-998-1 (ISBN)
Public defence
2011-06-01, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (Swedish)
Opponent
Supervisors
Funder
Swedish Research Council
Note
QC 20110516Available from: 2011-05-16 Created: 2011-05-13 Last updated: 2012-03-12Bibliographically approved

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