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Nanoarchitecturing of Natural Melanin Nanospheres by Layer-by-Layer Assembly: Macroscale Anti-inflammatory Conductive Coatings with Optoelectronic Tunability
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    Nanoarchitecturing of Natural Melanin Nanospheres by Layer-by-Layer Assembly: Macroscale Anti-inflammatory Conductive Coatings with Optoelectronic Tunability
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    Department of Chemical Engineering and Department of Polymer Science and Engineering, Inha University, 100 Inha-ro, Nam-gu, Incheon, Korea
    § Department of Materials Science and Engineering, University of Delaware, 201 Du Pont Hall, Newark Delaware 19716, United States
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    Biomacromolecules

    Cite this: Biomacromolecules 2017, 18, 6, 1908–1917
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    https://doi.org/10.1021/acs.biomac.7b00336
    Published May 16, 2017
    Copyright © 2017 American Chemical Society

    Abstract

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    Natural melanins are biocompatible conductors with versatile functionalities. Here, we report fabrication of multifunctional poly(vinyl alcohol)/melanin nanocomposites by layer-by-layer (LBL) assembly using melanin nanoparticles (MNPs) directly extracted from sepia officinalis inks. The LBL assembly offers facile manipulation of nanotextures as well as nm-thickness control of the macroscale film by varying solvent qualities. The time-resolved absorption was monitored during the process and quantitatively studied by fractal dimension and lacunarity analysis. The capability of nanoarchitecturing provides confirmation of complete monolayer formation and leads to tunable iridescent reflective colors of the MNP films. In addition, the MNP films have durable electrochemical conductivities as evidenced by enhanced charge storage capacities for 1000 cycles. Moreover, the MNP covered ITO (indium tin oxide) substrates significantly reduced secretion of inflammatory cytokines, TNF-α, by raw 264.7 macrophage cells compared to bare ITO, by a factor of 5 and 1.8 with and without lipopolysaccharide endotoxins, respectively. These results highlight the optoelectronic device-level tunability along with the anti-inflammatory biocompatibility of the MNP LBL film. This combination of performance should make these films particularly interesting for bioelectronic device applications such as electroceuticals, artificial bionic organs, biosensors, and implantable devices.

    Copyright © 2017 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.biomac.7b00336.

    • SEM images of MNP LBL assemblies; color-coded maps of local connected fractal dimension; SEM images of MNP LBL films; thickness controllability of MNP LBL films; cyclic voltammetry of a MNP LBL film assembled on ITO glass; UV–vis absorbance spectra during layering of MNP LBL films on an ITO glass; PC12 cell attachments results (PDF)

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    Biomacromolecules

    Cite this: Biomacromolecules 2017, 18, 6, 1908–1917
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.biomac.7b00336
    Published May 16, 2017
    Copyright © 2017 American Chemical Society

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