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Redox- and pH-Responsive Polymersomes with Ferrocene Moieties Exhibiting Peroxidase-like, Chemoenzymatic Activity and H2O2-Responsive Release Behavior

  • Silvia Moreno
    Silvia Moreno
    Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Straße 6, Dresden 01069, Germany
  • Hanna Hübner
    Hanna Hübner
    Polymer Chemistry, Saarland University, Campus Saarbrücken C4 2, Saarbrücken 66123, Germany
  • Christiane Effenberg
    Christiane Effenberg
    Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Straße 6, Dresden 01069, Germany
  • Susanne Boye
    Susanne Boye
    Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Straße 6, Dresden 01069, Germany
    More by Susanne Boye
  • Anthony Ramuglia
    Anthony Ramuglia
    Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany
  • Deborah Schmitt
    Deborah Schmitt
    Polymer Chemistry, Saarland University, Campus Saarbrücken C4 2, Saarbrücken 66123, Germany
  • Brigitte Voit
    Brigitte Voit
    Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Straße 6, Dresden 01069, Germany
    Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany
  • Inez M. Weidinger
    Inez M. Weidinger
    Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden 01062, Germany
  • Markus Gallei*
    Markus Gallei
    Polymer Chemistry, Saarland University, Campus Saarbrücken C4 2, Saarbrücken 66123, Germany
    Saarene, Saarland Center for Energy Materials and Sustainability, Campus C4 2, Saarbrücken 66123, Germany
    *Email: [email protected]
  • , and 
  • Dietmar Appelhans*
    Dietmar Appelhans
    Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Straße 6, Dresden 01069, Germany
    *Email: [email protected]
Cite this: Biomacromolecules 2022, 23, 11, 4655–4667
Publication Date (Web):October 10, 2022
https://doi.org/10.1021/acs.biomac.2c00901
Copyright © 2022 American Chemical Society

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    Abstract

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    The development of compartments for the design of cascade reactions in a local space requires a selective spatiotemporal control. The combination of enzyme-loaded polymersomes with enzymelike units shows a great potential in further refining the diffusion barrier and the type of reactions in nanoreactors. Herein, pH-responsive and ferrocene-containing block copolymers were synthesized to realize pH-stable and multiresponsive polymersomes. Permeable membrane, peroxidase-like behavior induced by the redox-responsive ferrocene moieties and release properties were validated using cyclovoltammetry, dye TMB assay, and rupture of host–guest interactions with β-cyclodextrin, respectively. Due to the incorporation of different block copolymers, the membrane permeability of glucose oxidase-loaded polymersomes was changed by increasing extracellular glucose concentration and in TMB assay, allowing for the chemoenzymatic cascade reaction. This study presents a potent synthetic, multiresponsive nanoreactor platform with tunable (e.g., redox-responsive) membrane properties for potential application in therapeutics.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.biomac.2c00901.

    • Characterization methods, synthesis and characterization of monomers and cross-linkers, further data on zeta potential, DLS, and stability of FcPsomes, host–guest interactions of FcPsomes, synthesis of FITC-GOx, conformation studies by AF4-LS, thermal analysis of BCPs, additional figures and tables for the characterization (NMR, cryo-TEM, CV, DLS, etc.) of monomers, BCPs, and FcPsomes (PDF)

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    Cited By

    This article is cited by 5 publications.

    1. Ting Liu, Liwei Zhu, Chencan Li, Yang Yu, Zhuo Zhang, Huizhong Liu, Ling Wang, Yawen Li. Fe-CP-based Catalytic Oxidation and Dissipative Self-Assembly of a Ferrocenyl Surfactant Applied in DNA Capture and Release. ACS Omega 2024, 9 (22) , 23772-23781. https://doi.org/10.1021/acsomega.4c01715
    2. Nayeong Kim, Wangsuk Oh, Kyle N. Knust, Fábio Zazyki Galetto, Xiao Su. Molecularly Selective Polymer Interfaces for Electrochemical Separations. Langmuir 2023, 39 (47) , 16685-16700. https://doi.org/10.1021/acs.langmuir.3c02389
    3. Deborah Schmitt, Salma M. Abdel-Hafez, Marco Tummeley, Volker Schünemann, Marc Schneider, Volker Presser, Markus Gallei. Surface-Initiated Living Anionic Polymerization of Functional Methacrylates from the Surface of Organic Particles. Macromolecules 2023, 56 (17) , 7086-7101. https://doi.org/10.1021/acs.macromol.3c01257
    4. Xiangyang Zhang, Yinghao Ding, Zhenghao Zhang, Yiping Ma, Xuan Sun, Ling Wang, Zhimou Yang, Zhi-Wen Hu. In Situ Construction of Ferrocene-Containing Membrane-Bound Nanofibers for the Redox Control of Cancer Cell Death and Cancer Therapy. Nano Letters 2023, 23 (16) , 7665-7674. https://doi.org/10.1021/acs.nanolett.3c02362
    5. Dishi Wang, Silvia Moreno, Susanne Boye, Brigitte Voit, Dietmar Appelhans. Crosslinked and Multi‐Responsive Polymeric Vesicles as a Platform to Study Enzyme‐Mediated Undocking Behavior: Toward Future Artificial Organelle Communication. Macromolecular Rapid Communications 2023, 18 , 2200885. https://doi.org/10.1002/marc.202200885