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Characterization of glycopolymers by asymmetric flow field-flow fractionation

dc.contributor.advisorPasch, Haralden_ZA
dc.contributor.advisorLederer, Albenaen_ZA
dc.contributor.authorWilliams, Chelsea Danielleen_ZA
dc.contributor.otherStellenbosch University. Faculty of Science. Dept. of Chemistry and Polymer Science.en_ZA
dc.date.accessioned2020-12-01T05:57:14Z
dc.date.accessioned2021-01-31T19:36:00Z
dc.date.available2020-12-01T05:57:14Z
dc.date.available2021-01-31T19:36:00Z
dc.date.issued2020-12
dc.identifier.urihttp://hdl.handle.net/10019.1/109116
dc.descriptionThesis (MSc)--Stellenbosch University, 2020.en_ZA
dc.description.abstractENGLISH ABSTRACT: An alternative route for studying the interactions between human serum albumin (HSA) and dendronized glycopolymers was implemented by applying a versatile asymmetric flow field-flow fractionation (AF4) technique. Dendronized polymers (DenPols) decorated with maltose moieties, have an abundance of hydrogen bonding sites that isdesirable for interactions with HSA. The difficulty with the characterization of lysine maleimide DenPols and poly(ethylene glycol) (PEG) maleimide DenPols arethe ultrahigh molar masses and the molecular heterogeneity. Here, we aimed to apply the gentle AF4 technique in combination with a refractive index and light scattering detectorsto comprehensively characterize the lysine maleimide DenPols decorated with a maltose shell (MI-G0-MAL –MI-G3-MAL), PEG maleimide DenPol (MI-G1-PEG-MAL), human serum albumin (HSA) and complexes formed by the interaction of DenPols andHSA. An in-depthanalysis of the DenPols,regarding theirmolar mass distribution, radiusof gyration,hydrodynamic radius, dispersity,and molecular architecturewas conducted. The determination of these properties wasexamined using batch mode dynamic light scattering (DLS), size exclusion chromatography (SEC) and AF4. Bothseparation techniques explicitly showed the pronounced aggregation of the DenPols. AF4 showed the DenPols being present assingle macromolecules with arandom coil conformationand aggregatesas elongated (rod-like) or spherical conformations. Complexes formed between DenPols and HSA showed a deviation in the aggregation mechanism compared to the individual DenPols, as the conformation of the non-aggregated and aggregated structures were different. The complexation behaviour between DenPols and HSA displayedaggregated structures of hard dense spherical and swollen moleculararchitectures. MI-G3-MAL with more available hydrogen bonding sites showed significant changes in the conformation when interacting with HSA. The study demonstrated that the multivalentinteractions of DenPols with HSA indicate the tunable aggregation and conformation of DenPols.en_ZA
dc.description.abstractAFRIKAANSE OPSOMMING: ‘nAlternatiewestudieroete is gevolg vir die bestudering vandie interaksie tussen menslike serumalbumien (HSA) en gedendroniseer glikopolymere. Dit was geimplementeer deur die toepassing van‘n veelsydige onsimmetriese vloei-veldvloeifraksioneringtegniek (AF4). Gedendroniseerdepolymere(DenPols) versier (gelaai) met maltose eindgroepe, het’n magdom (verskeidenheid)van waterstofbindingswerwewat voordelig isvirinteraksiesvan HSA. Die uitdaging met die karaktarisering van lysienmaleimiedDenPols en poli(etileenglikol)(PEG)maleimiedDenPols, is die ultrahoë molêre eenhedeen die molekulêre heterogeniteit. Hier het onsgepoog om toepassing van die sagte AF4 tegniek inkombinasie met ‘nrefraktiewe indeks en ligte verspreiders aan te wend. Hierdeur kon ons die lysine maleimide wat versier is met maltose bedecking ( MI-G0-MAL -MI-G3-MAL), PEG maleimide DenPol (MI-G1-PEG-MAL), HSA en komplekse wat ontstaan het deur die interaksie van DenPols en HSA omvattend karakteriseer.‘n In diepte analise van DenPols aangaande hul “molar” massa verspreiding radius of omwenteling, hidrodinamiese verspreiding en molekulêre argitektuur was uitgevoer. Die vasberadenheid van hierdie elemente is aangedui deur die gebruik van bondelmodus dinamiese ligverspreiding (DLS), grootte-uitsluitschromatografie (SEC) en AF4 tegniek. Beide skeidingstegnieke het baie duidelik die samevoeging van DenPols gedui. AF4 lewer bewys dat DenPols teenwoordig is as ‘n enkele makromolekule met ‘n willekeurige spoelstruktuur en ‘n samevoeging as ‘n verlengde staaf of sferise struktuur. Komplekse wat gevorm is tussen DenPols en HSA het ‘n afwyking met die aggressie meganisme in vergelyking met die individuele DenPols aangesien die ooreenkomstigheid van die saamgestelde en nie saamgestelde structure verskillend was. Die komplekse gedrag tussen DenPols en HSA het samegestelde structure van harde, digte sferiese en geswolle molekulêre argitektuur. MI-G3-MAL het beskikbare waterstofverbonde werwe getoon wat beduidende veranderinge getoon het wanneer dit met HSA in interaksie is. Die studie illustreer dus die multivalente interaksie van DenPols met HSA asook die afstembare samevoeging en ooreenkomstigheid van DenPols.af_ZA
dc.format.extent116 pagesen_ZA
dc.language.isoen_ZAen_ZA
dc.publisherStellenbosch : Stellenbosch Universityen_ZA
dc.subjectDendronized glycopolymersen_ZA
dc.subjectAsymmetry (Chemistry)en_ZA
dc.subjectUCTDen_ZA
dc.subjectFractionation, Field-flowen_ZA
dc.titleCharacterization of glycopolymers by asymmetric flow field-flow fractionationen_ZA
dc.typeThesisen_ZA
dc.description.versionMastersen_ZA
dc.rights.holderStellenbosch Universityen_ZA


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