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Spatiotemporal Control of Melanin Synthesis in Liquid Droplets

  • Tlalit Massarano
    Tlalit Massarano
    Shmunis School of Biomedicine and Cancer Research, George S. Wise Faculty of Life Sciences, Tel Aviv University, Tel Aviv 69978, Israel
  • Avigail Baruch Leshem
    Avigail Baruch Leshem
    Shmunis School of Biomedicine and Cancer Research, George S. Wise Faculty of Life Sciences, Tel Aviv University, Tel Aviv 69978, Israel
  • Michal Weitman
    Michal Weitman
    Department of Chemistry, Bar -Ilan University, Ramat-Gan 5290002, Israel
  • , and 
  • Ayala Lampel*
    Ayala Lampel
    Shmunis School of Biomedicine and Cancer Research, George S. Wise Faculty of Life Sciences, Tel Aviv University, Tel Aviv 69978, Israel
    Center for Nanoscience and Nanotechnology, Tel Aviv University, Tel Aviv 69978, Israel
    Sagol Center for Regenerative Biotechnology, Tel Aviv University, Tel Aviv 69978, Israel
    Center for the Physics and Chemistry of Living Systems, Tel Aviv University, Tel Aviv 69978, Israel
    *Email: [email protected]
    More by Ayala Lampel
Cite this: ACS Appl. Mater. Interfaces 2022, 14, 18, 20520–20527
Publication Date (Web):April 22, 2022
https://doi.org/10.1021/acsami.1c21006
Copyright © 2022 American Chemical Society

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    Abstract

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    Melanins are natural biopolymers that have remarkable properties including UV-protection, coloration, and antioxidant activity. Their biosynthesis is regulated both spatially and temporally and involves supramolecular templating and compartmentalization of enzymes and reactants within specialized organelles called melanosomes. In contrast, the laboratory-based bulk synthesis of melanin by tyrosine or dopamine oxidation is a poorly controlled process, resulting in materials with undefined properties. Inspired by the pigment’s biosynthesis, we developed a methodology to spatiotemporally regulate melanin formation in liquid droplets. The spatial control is achieved by sequestration of the reaction in dextran-rich droplets of a polyethylene glycol/dextran aqueous two-phase system, where the use of a photocleavable protected tyrosine provides a temporal control over its enzymatic oxidation–polymerization. We show that the liquid droplets allow for confined local reactivity as they serve as reaction centers for melanin synthesis and compartmentalize the melanin product. This methodology opens tremendous opportunities for applications in skincare and biomedicine.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c21006.

    • HPLC analysis of ONB-Y cleavage; UV–vis spectroscopy analysis of melanin in droplets; macroscopic images, confocal microscopy images, and TEM micrographs of melanin in PEG/Dex droplets; ToF-SIMS analysis of the melanin formed in droplets (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Qiang Zhang, Tianze Xie, Xizhen Yi, Gaowa Xing, Shuo Feng, Shulang Chen, Yuxuan Li, Jin-Ming Lin. Microfluidic Aqueous Two-Phase Focusing of Chemical Species for In Situ Subcellular Stimulation. ACS Applied Materials & Interfaces 2023, 15 (39) , 45640-45650. https://doi.org/10.1021/acsami.3c09665

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