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Probing Crowdedness of Artificial Organelles by Clustering Polymersomes for Spatially Controlled and pH-Triggered Enzymatic Reactions

  • Peng Wang
    Peng Wang
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    Organic Chemistry of Polymers, Technische Universität Dresden, D-01062 Dresden, Germany
    More by Peng Wang
  • Silvia Moreno*
    Silvia Moreno
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    *E-mail [email protected]; Tel 49-351-4658494; Fax 49-3514658565.
  • Andreas Janke
    Andreas Janke
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
  • Susanne Boye
    Susanne Boye
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    More by Susanne Boye
  • Dishi Wang
    Dishi Wang
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    Organic Chemistry of Polymers, Technische Universität Dresden, D-01062 Dresden, Germany
    More by Dishi Wang
  • Simona Schwarz
    Simona Schwarz
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
  • Brigitte Voit
    Brigitte Voit
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    Organic Chemistry of Polymers, Technische Universität Dresden, D-01062 Dresden, Germany
  • , and 
  • Dietmar Appelhans*
    Dietmar Appelhans
    Leibniz Institute for Polymer Research Dresden, Hohe Strasse 6, D-01069 Dresden, Germany
    *E-mail [email protected]; Tel 49-351-4658353; Fax 49-3514658565.
Cite this: Biomacromolecules 2022, 23, 9, 3648–3662
Publication Date (Web):August 18, 2022
https://doi.org/10.1021/acs.biomac.2c00546
Copyright © 2022 American Chemical Society

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    Abstract

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    Most sophisticated biological functions and features of cells are based on self-organization, and the coordination and connection between their cell organelles determines their key functions. Therefore, spatially ordered and controllable self-assembly of polymersomes to construct clusters to simulate complex intracellular biological functions has attracted widespread attention. Here, we present a simple one-step copper-free click strategy to cross-link nanoscale pH-responsive and photo-cross-linked polymersomes (less than 100 nm) to micron-level clusters (more than 90% in 0.5–2 μm range). Various influencing factors in the clustering process and subsequent purification methods were studied to obtain optimal clustered polymeric vesicles. Even when polymeric vesicles separately loaded with different enzymes (glucose oxidase and myoglobin) are coclustered, the overall permeability of the clusters can still be regulated through tuning the pH values on demand. Compared with simple blending of those enzyme-loaded polymersomes, the rate of enzymatic cascade reaction increased significantly due to the interconnected complex microstructure established. The connection of catalytic nanocompartments into clusters confining different enzymes of a cascade reaction provides an excellent platform for the development of artificial systems mimicking natural organelles or cells.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.biomac.2c00546.

    • Characterization methods, synthetic procedure of block copolymers and bis-cyclooctyne cross-linker, corresponding NMR data, additional Cryo-TEM images of Psomes and clustered Psomes, TEM images of clustered Psomes, DLS data for tracking clustering process, in situ AFM images and cross-section, histogram of the size distribution of clustered Psomes, enzyme activity characterization, AF4 fractograms (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 1 publications.

    1. Giovanni B. Perin, Silvia Moreno, Yang Zhou, Markus Günther, Susanne Boye, Brigitte Voit, Maria I. Felisberti, Dietmar Appelhans. Construction of Membraneless and Multicompartmentalized Coacervate Protocells Controlling a Cell Metabolism-like Cascade Reaction. Biomacromolecules 2023, 24 (12) , 5807-5822. https://doi.org/10.1021/acs.biomac.3c00828