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    Rheology of Block Copolypeptide Solutions:  Hydrogels with Tunable Properties
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    Materials Research Laboratory, Department of Chemical Engineering, and Departments of Materials and Chemistry, University of California, Santa Barbara, California 93106 and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332
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    Macromolecules

    Cite this: Macromolecules 2004, 37, 10, 3943–3953
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    https://doi.org/10.1021/ma049885f
    Published April 24, 2004
    Copyright © 2004 American Chemical Society
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    Abstract

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    Amphiphilic block copolypeptides were prepared through transition-metal-mediated polymerization of amino acid N-carboxyanhydrides. In aqueous solution these materials form strong hydrogels at low concentrations. The self-assembly process that is responsible for gelation was investigated by measuring the rheological properties of the gels for a variety of molecular architectures:  poly-l-lysine-b-poly-l-leucine diblock and poly-l-lysine-b-poly-l-leucine-b-poly-l-lysine triblock copolypeptides. Experiments showed that the rodlike helical secondary structure of enantiomerically pure poly-l-leucine blocks was instrumental for gelation at polypeptide concentrations as low as 0.25 wt %. The hydrophilic polyelectrolyte segments have stretched coil configurations and stabilize the twisted fibril assemblies by forming a corona around the hydrophobic core. The self-assembly of hydrophobic blocks is highly specific and sensitive to the chirality of the helices. It was found that mechanical properties of the gels can be tuned through the molecular architecture of the block copolypeptides and also by carefully mixing different polypeptides in solution.

    Copyright © 2004 American Chemical Society

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     To whom correspondence should be addressed. E-mail: [email protected].

    †

     Materials Research Laboratory, University of California, Santa Barbara.

    ‡

     Department of Chemical Engineering, University of California, Santa Barbara.

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     Georgia Institute of Technology.

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     Departments of Materials and Chemistry, University of California, Santa Barbara.

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    Macromolecules

    Cite this: Macromolecules 2004, 37, 10, 3943–3953
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    https://doi.org/10.1021/ma049885f
    Published April 24, 2004
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