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Chain-Folding and Overall Molecular Conformation in a Novel Amphiphilic Starlike Macromolecule

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Polymer Program, Institute of Materials Science and Department of Chemical Engineering, The University of Connecticut, Storrs, Connecticut 06269-3136; Baker Laboratory of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853; Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, New Jersey 08854; Chemistry Department, State University of New York at Stony Brook, Stony Brook, New York 11794; and Polymer Program, Institute of Materials Science and Department of Physics, The University of Connecticut, Storrs, Connecticut 06269
Cite this: Macromolecules 2005, 38, 16, 7074–7082
Publication Date (Web):July 9, 2005
https://doi.org/10.1021/ma050983q
Copyright © 2005 American Chemical Society

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    Abstract

    The crystallization and self-assembly behavior of an amphiphilic starlike macromolecule (ASM) with a lipophilic core and four poly(ethylene oxide) (PEO) arms (Mn = 2000 g/mol) were characterized by synchrotron small-angle X-ray scattering (SAXS) and wide-angle X-ray diffraction at different crystallization temperatures (Tc). The overall d-spacing of the alternating amorphous core and crystalline PEO lamellae almost doubled from 11.4 nm for samples quenched into liquid nitrogen to 21.0 nm for Tc = 42 °C, indicating gradual transitions from nearly once-folded to fractionally folded and finally to extended chain crystals with increasing the Tc. On the basis of SAXS, transmission electron microscopy, and computer simulation results, it was suggested that the lamellae contained an interdigitated, single-layered PEO crystal, and an amorphous layer consisted of a double-layered lipophilic core and amorphous PEO. A folded (four PEO arms at one side of the core) rather than an extended (two PEO arms on each side of the core) overall molecular conformation (OMC) of the ASM was deduced in the solid state. These results implied that chain-folding and OMC of the ASM closely depended on its star-block-like architecture.

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     Institute of Materials Science and Department of Chemical Engineering, The University of Connecticut.

     Cornell University.

    *

     Corresponding author:  e-mail [email protected]; Tel 860-486-8708.

    §

     Rutgers University.

     State University of New York at Stony Brook.

    #

     Institute of Materials Science and Department of Physics, The University of Connecticut.

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