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Polyglycerol-Based Thermoresponsive Nanocapsules Induce Skin Hydration and Serve as a Skin Penetration Enhancer

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    Biological and Medical Applications of Materials and Interfaces

    Polyglycerol-Based Thermoresponsive Nanocapsules Induce Skin Hydration and Serve as a Skin Penetration Enhancer
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    • Ernesto R. Osorio-Blanco
      Ernesto R. Osorio-Blanco
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Takustr. 3, 14195 Berlin, Germany
      More by Ernesto R. Osorio-Blanco
      Orcidhttp://orcid.org/0000-0002-9279-6813
    • Fiorenza Rancan
      Fiorenza Rancan
      Clinical Research Center for Hair and Skin Science, Department of Dermatology and Allergy, Charité—Universitätsmedizin Berlin, Charitéplatz 1, 10117 Berlin, Germany
      More by Fiorenza Rancan
      Orcidhttp://orcid.org/0000-0003-3903-3240
    • André Klossek
      André Klossek
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Arnimallee 22, 14195 Berlin, Germany
      More by André Klossek
    • Jan H. Nissen
      Jan H. Nissen
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Fabeckstr. 34/36, 14195 Berlin, Germany
      More by Jan H. Nissen
    • Luisa Hoffmann
      Luisa Hoffmann
      Clinical Research Center for Hair and Skin Science, Department of Dermatology and Allergy, Charité—Universitätsmedizin Berlin, Charitéplatz 1, 10117 Berlin, Germany
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    • Julian Bergueiro
      Julian Bergueiro
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Takustr. 3, 14195 Berlin, Germany
      Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CIQUS), Departamento de Química Orgánica, Universidade de Santiago de Comopostela, 15782 Santiago de Compostela, Spain
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      Orcidhttp://orcid.org/0000-0001-8700-0000
    • Sebastian Riedel
      Sebastian Riedel
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Fabeckstr. 34/36, 14195 Berlin, Germany
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    • Annika Vogt
      Annika Vogt
      Clinical Research Center for Hair and Skin Science, Department of Dermatology and Allergy, Charité—Universitätsmedizin Berlin, Charitéplatz 1, 10117 Berlin, Germany
      More by Annika Vogt
    • Eckart Rühl
      Eckart Rühl
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Arnimallee 22, 14195 Berlin, Germany
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      Orcidhttp://orcid.org/0000-0002-0451-8734
    • Marcelo Calderón*
      Marcelo Calderón
      Freie Universität Berlin, Institute of Chemistry and Biochemistry, Takustr. 3, 14195 Berlin, Germany
      POLYMAT and Applied Chemistry Department, Faculty of Chemistry, University of the Basque Country, UPV/EHU, Paseo Manuel de Lardizabal 3, 20018 Donostia-San Sebastián, Spain
      IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Spain
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0002-2734-9742
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 27, 30136–30144
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    https://doi.org/10.1021/acsami.0c06874
    Published June 10, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    The use of penetration enhancers (chemical or physical) has been proven to dramatically improve the penetration of therapeutics. Nevertheless, their use poses great risks, as they can lead to permanent damage of the skin, reduce its barrier efficiency, and result in the intrusion of harmful substances. Among the most used skin penetration enhancers, water is greatly accepted because skin quickly recovers from its exposure. Nanocapsules (NCs) represent a promising combination of the carrier system and penetration enhancer because their water-containing void combined with their polymer-based shell can be used to induce high local skin hydration, while simultaneously aiding the transport of drugs across the skin barrier. In this study, NCs were synthesized with a void core of 100 nm in diameter, a thermoresponsive shell based on different ratios of poly(N-isopropylacrylamide) and poly(N-isopropylmethacrylamide) as thermoresponsive polymers, and dendritic polyglycerol as a macromolecular cross-linker. These NCs can shrink or swell upon a thermal trigger, which was used to induce the release of the entrapped water in a controlled fashion. The interactions and effects of thermoresponsive NCs on the stratum corneum of excised human skin were investigated using fluorescence microscopy, high-resolution optical microscopy, and stimulated Raman spectromicroscopy. It could be observed that the thermoresponsive NCs increase the amount of deuterated water that penetrated into the viable epidermis. Moreover, NCs increased the skin penetration of a high-molecular weight dye (Atto Oxa12 NHS ester, MW = 835 g/mol) with respect to formulations in water or 30% DMSO, emphasizing the features of the NCs as a skin penetration enhancer.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c06874.

    • Reaction conditions of the screening for yielding dPG-PNIPAM SiO2@NGs, 1H-NMR spectra from selected results from synthetic screenings, height image and (A) deformation map of dPG-PNIPAM (B), SiO2@NGs imaged by AFM, TEM images of dPG-PNIPAM-co-PNIPMAM (1:1) (A) SiO2@NGs and (B) NCs, and (A) height image and (B) deformation map of dPG-PNIPAM-co-PNIPMAM (1:1) NCs imaged by AFM (PDF)

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    This article is cited by 14 publications.

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    9. Mahdiyar Shahbazi, Henry Jäger, Rammile Ettelaie, Adeleh Mohammadi, Peyman Asghartabar Kashi. Multimaterial 3D printing of self-assembling smart thermo-responsive polymers into 4D printed objects: A review. Additive Manufacturing 2023, 71 , 103598. https://doi.org/10.1016/j.addma.2023.103598
    10. Neha Tiwari, Ernesto Rafael Osorio‐Blanco, Ana Sonzogni, David Esporrín‐Ubieto, Huiyi Wang, Marcelo Calderón. Nanocarriers for Skin Applications: Where Do We Stand?. Angewandte Chemie 2022, 134 (3) https://doi.org/10.1002/ange.202107960
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    12. Tisana Kaewruethai, Chavee Laomeephol, Yue Pan, Jittima Amie Luckanagul. Multifunctional Polymeric Nanogels for Biomedical Applications. Gels 2021, 7 (4) , 228. https://doi.org/10.3390/gels7040228
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    14. Louise Van Gheluwe, Igor Chourpa, Coline Gaigne, Emilie Munnier. Polymer-Based Smart Drug Delivery Systems for Skin Application and Demonstration of Stimuli-Responsiveness. Polymers 2021, 13 (8) , 1285. https://doi.org/10.3390/polym13081285
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 27, 30136–30144
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c06874
    Published June 10, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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