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    Side-chain-controlled self-assembly of polystyrene-polypeptide miktoarm star copolymers

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    Type
    Article
    Authors
    Junnila, Susanna
    Houbenov, Nikolay
    Karatzas, A.
    Hadjichristidis, Nikos cc
    Hirao, Akira
    Iatrou, Hermis
    Ikkala, Olli T.
    KAUST Department
    Biological and Environmental Sciences and Engineering (BESE) Division
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Polymer Synthesis Laboratory
    Date
    2012-03-07
    Online Publication Date
    2012-03-07
    Print Publication Date
    2012-03-27
    Permanent link to this record
    http://hdl.handle.net/10754/562136
    
    Metadata
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    Abstract
    We show how the self-assembly of miktoarm star copolymers can be controlled by modifying the side chains of their polypeptide arms, using A 2B and A 2B 2 type polymer/polypeptide hybrids (macromolecular chimeras). Initially synthesized PS 2PBLL and PS 2PBLL 2 (PS, polystyrene; PBLL, poly(ε-tert-butyloxycarbonyl-l-lysine) ) miktoarms were first deprotected to PS 2PLLHCl and PS 2PLLHCl 2 miktoarms (PLLHCl, poly(l-lysine hydrochloride)) and then complexed ionically with sodium dodecyl sulfonate (DS) to give the supramolecular complexes PS 2PLL(DS) and PS 2(PLL(DS)) 2. The solid-state self-assemblies of these six miktoarm systems were studied by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and small- and wide-angle X-ray scattering (SAXS, WAXS). The side chains of the polypeptide arms were observed to have a large effect on the solubility, polypeptide conformation, and self-assembly of the miktoarms. Three main categories were observed: (i) lamellar self-assemblies at the block copolymer length scale with packed layers of α-helices in PS 2PBLL and PS 2PBLL 2; (ii) charge-clustered polypeptide micelles with less-defined conformations in a nonordered lattice within a PS matrix in PS 2PLLHCl and PS 2PLLHCl 2; (iii) lamellar polypeptide-surfactant self-assemblies with β-sheet conformation in PS 2PLL(DS) and PS 2(PLL(DS)) 2 which dominate over the formation of block copolymer scale structures. Differences between the 3- and 4-arm systems illustrate how packing frustration between the coil-like PS arms and rigid polypeptide conformations can be relieved by the right number of arms, leading to differences in the extent of order. © 2012 American Chemical Society.
    Citation
    Junnila, S., Houbenov, N., Karatzas, A., Hadjichristidis, N., Hirao, A., Iatrou, H., & Ikkala, O. (2012). Side-Chain-Controlled Self-Assembly of Polystyrene–Polypeptide Miktoarm Star Copolymers. Macromolecules, 45(6), 2850–2856. doi:10.1021/ma202747h
    Publisher
    American Chemical Society (ACS)
    Journal
    Macromolecules
    DOI
    10.1021/ma202747h
    ae974a485f413a2113503eed53cd6c53
    10.1021/ma202747h
    Scopus Count
    Collections
    Articles; Biological and Environmental Sciences and Engineering (BESE) Division; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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