Water-Dispersible Cationic Polyurethanes Containing Pendant Trialkylphosphoniums

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dc.contributorChemistryen
dc.contributorMacromolecules and Interfaces Institute at Virginia Techen
dc.contributor.authorZhang, Musanen
dc.contributor.authorHemp, Sean T.en
dc.contributor.authorZhang, Mingqiangen
dc.contributor.authorAllen, Michael H. Jr.en
dc.contributor.authorCarmean, Richard N.en
dc.contributor.authorMoore, Robert Bowenen
dc.contributor.authorLong, Timothy E.en
dc.contributor.departmentChemistryen
dc.date.accessed2015-04-16en
dc.date.accessioned2015-04-20T18:49:34Zen
dc.date.available2015-04-20T18:49:34Zen
dc.date.issued2014-03-06en
dc.description.abstractNovel trialkylphosphonium ionic liquids chain extenders enabled the successful synthesis of poly(ethylene glycol)-based, cationic polyurethanes with pendant phosphoniums in the hard segments (HS). Aqueous size exclusion chromatography (SEC) confirmed the charged polyurethanes, which varied the phosphonium alkyl substituent length (ethyl and butyl) and cationic HS content (25, 50, 75 mol%), achieved high absolute molecular weights. Dynamic mechanical analysis (DMA) demonstrated the triethylphosphonium (TEP) and tributylphosphonium (TBP) polyurethanes displayed similar thermomechanical properties, including increased rubbery plateau moduli and flow temperatures. Fourier transform infrared spectroscopy (FTIR) emphasized the significance of ion_dipole interaction on hydrogen bonding. Atomic force microscopy (AFM), small-angle X-ray scattering (SAXS), and wide-angle X-ray diffraction (WAXD) supported microphase separated morphologies in the trialkylphosphonium polyurethanes, despite the presence of ionic interactions. Sorption isotherm experiments revealed the TEP polyurethane exhibited the highest water vapor sorption profile compared to the TBP, which displayed similar water sorption profiles to the noncharged analogue. The phosphonium polyurethanes displayed significantly improved tensile strain; however, lower tensile stress of the TEP polyurethane was presumably due to absorbed water. In addition to physical characterizations, we also explored the trialkylphosphonium polyurethanes as nucleic acid delivery vectors. The phosphonium polyurethanes bound DNA at low charge ratios, and the polyplexes exhibited enhanced colloidal stability under physiological salt conditions.en
dc.description.notesSupplementary information is included in a separate fileen
dc.description.sponsorshipU.S. Army Research Laboratory, Army Materials Center of Excellence Programen
dc.description.sponsorshipUnited States. Army Research Office - Contract W911NF-06-2-0014en
dc.description.sponsorshipUnited States. Army Research Office - Grant no. W911NF-07-1-0452 Ionic Liquids in Electro-active Devices (ILEAD) MURIen
dc.description.sponsorshipNational Science Foundation (U.S.) - Grant no. DMR-0923107en
dc.description.sponsorshipBayer Material Scienceen
dc.format.mimetypeapplication/pdfen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationZhang, M., Hemp, S. T., Zhang, M., Allen, M. H., Carmean, R. N., Moore, R. B., & Long, T. E. (2014). Water-dispersible cationic polyurethanes containing pendant trialkylphosphoniums. Polymer Chemistry, 5(12), 3795-3803. doi: 10.1039/C3PY01779Fen
dc.identifier.doihttps://doi.org/10.1039/C3PY01779Fen
dc.identifier.issn1759-9954en
dc.identifier.urihttp://hdl.handle.net/10919/51700en
dc.identifier.urlhttp://pubs.rsc.org/en/content/articlelanding/2014/py/c3py01779fen
dc.language.isoen_USen
dc.publisherThe Royal Society of Chemistryen
dc.rightsCreative Commons Attribution-NonCommercial 3.0 Unporteden
dc.rights.urihttp://creativecommons.org/licenses/by-nc/3.0/en
dc.subjectMacromolecular designen
dc.subjectTrialkylphosphonium diol synthesisen
dc.subjectPolyurethane synthesisen
dc.subjectCationic polyurethanesen
dc.titleWater-Dispersible Cationic Polyurethanes Containing Pendant Trialkylphosphoniumsen
dc.title.serialPolymer Chemistryen
dc.typeArticle - Refereeden
dc.typeDataseten
dc.type.dcmitypeTexten
dc.type.dcmitypeDataseten

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