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Polyampholytic Poly(dehydroalanine) Graft Copolymers as Smart Templates for pH-Controlled Formation of Alloy Nanoparticles

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    Polyampholytic Poly(dehydroalanine) Graft Copolymers as Smart Templates for pH-Controlled Formation of Alloy Nanoparticles
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    • J. B. Max
      J. B. Max
      Institute of Organic Chemistry and Macromolecular Chemistry (IOMC), Friedrich-Schiller-University Jena, Lessingstraße 8, D-07743 Jena, Germany
      Jena Center for Soft Matter (JCSM), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Center for Energy and Environmental Chemistry (CEEC), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      More by J. B. Max
    • K. Kowalczuk
      K. Kowalczuk
      Institute of Organic Chemistry and Macromolecular Chemistry (IOMC), Friedrich-Schiller-University Jena, Lessingstraße 8, D-07743 Jena, Germany
      Jena Center for Soft Matter (JCSM), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Center for Energy and Environmental Chemistry (CEEC), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      More by K. Kowalczuk
    • M. Köhler
      M. Köhler
      Institute of Organic Chemistry and Macromolecular Chemistry (IOMC), Friedrich-Schiller-University Jena, Lessingstraße 8, D-07743 Jena, Germany
      More by M. Köhler
    • C. Neumann
      C. Neumann
      Jena Center for Soft Matter (JCSM), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Center for Energy and Environmental Chemistry (CEEC), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Institute of Physical Chemistry (IPC), Friedrich-Schiller-University Jena, Lessingstraße 10, D-07743 Jena, Germany
      More by C. Neumann
    • F. Pielenz
      F. Pielenz
      Institute of Organic Chemistry and Macromolecular Chemistry (IOMC), Friedrich-Schiller-University Jena, Lessingstraße 8, D-07743 Jena, Germany
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    • L. V. Sigolaeva
      L. V. Sigolaeva
      Department of Chemistry, M.V. Lomonosov Moscow State University, Leninskie Gory 1/3, 119991 Moscow, Russia
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    • D. V. Pergushov
      D. V. Pergushov
      Department of Chemistry, M.V. Lomonosov Moscow State University, Leninskie Gory 1/3, 119991 Moscow, Russia
      More by D. V. Pergushov
    • A. Turchanin
      A. Turchanin
      Jena Center for Soft Matter (JCSM), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Center for Energy and Environmental Chemistry (CEEC), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Institute of Physical Chemistry (IPC), Friedrich-Schiller-University Jena, Lessingstraße 10, D-07743 Jena, Germany
      More by A. Turchanin
      Orcidhttp://orcid.org/0000-0003-2388-1042
    • F. Langenhorst
      F. Langenhorst
      Institute of Geoscience, Friedrich-Schiller-University Jena, Carl-Zeiss-Promenade 10, D-07743 Jena, Germany
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    • F. H. Schacher*
      F. H. Schacher
      Institute of Organic Chemistry and Macromolecular Chemistry (IOMC), Friedrich-Schiller-University Jena, Lessingstraße 8, D-07743 Jena, Germany
      Jena Center for Soft Matter (JCSM), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      Center for Energy and Environmental Chemistry (CEEC), Friedrich-Schiller-University Jena, Philosophenweg 7, D-07743 Jena, Germany
      *Email: [email protected]
      More by F. H. Schacher
      Orcidhttp://orcid.org/0000-0003-4685-6608
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    Macromolecules

    Cite this: Macromolecules 2020, 53, 11, 4511–4523
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.0c00474
    Published May 20, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Polymer templates are a facile way to control the formation, size, and shape of different inorganic nanomaterials by tuning solution behavior, morphology, or density and the type of functional groups. As a novel class of such templates, we herein introduce polyampholytic graft copolymers, more specifically, poly(dehydroalanine)-graft-poly(ethylene glycol) (PDha-g-PEG), which feature a polyampholytic backbone with varying net charge and charge densities at different pH values and PEG grafts, providing molecular solubility over the entire pH range. As the PDha backbone features both amino and carboxylic acid groups in each repeat unit, selective interaction with [AuCl4]- and Ag+ salts is possible, and this permits a straightforward synthesis of Ag, Au, and AgAu alloy nanoparticles. In this regard, we used different approaches: light-induced, thermal, and chemical reduction. As a unique feature, PDha-g-PEG enables control over AgAu nanoalloy composition via the pH value, as this directly affects the charge ratio (−NH3+/–COO–) along the polymeric backbone. The obtained hybrid materials were investigated with respect to structure, shape, composition, and optical properties of nanoparticles via transmission electron microscopy, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy, thermogravimetric analysis, and UV–vis spectroscopy. In our opinion, this is a facile way to control nanoalloy composition and this can be extended to other mono- or bimetallic nanoparticle examples.

    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/acs.macromol.0c00474.

    • NMR, SEC traces, DLS curves, TEM micrographs, UV–vis spectrum, XPS overview, HR-TEM micrographs, and TGA curves (PDF)

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    This article is cited by 17 publications.

    1. Tolga Ceper, Daniel Costabel, Daniel Kowalczyk, Kalina Peneva, Felix H. Schacher. Noble Metal-Free Light-Driven Hydrogen Evolution Catalysis in Polyampholytic Hydrogel Networks. ACS Applied Materials & Interfaces 2024, 16 (19) , 24796-24805. https://doi.org/10.1021/acsami.4c04045
    2. Tolga Çeper, Afshin Nabiyan, Christof Neumann, Andrey Turchanin, Felix H. Schacher. Visible-Light-Driven Hydrogen Evolution of PtNP/[Ru(bpy)3]2+/Polyampholyte Hybrid Hydrogels. ACS Applied Polymer Materials 2023, 5 (8) , 6493-6503. https://doi.org/10.1021/acsapm.3c01051
    3. Daniel Costabel, Ratnadip De, Franz Jacobi, Jonas Eichhorn, Konrad Hotzel, Afshin Nabiyan, Christof Neumann, Andrey Turchanin, Stephan Kupfer, Felix H. Schacher, Sven Rau, Benjamin Dietzek-Ivanšić, Kalina Peneva. Bridging Platinum and Palladium to Bipyridine-Annulated Perylene for Light-Driven Hydrogen Evolution. ACS Catalysis 2023, 13 (11) , 7159-7169. https://doi.org/10.1021/acscatal.3c01201
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    5. Frieda Nagler, Christine Schiller, Christian Kropf, Felix H. Schacher. Amphiphilic Graft Copolymers for Time-Delayed Release of Hydrophobic Fragrances. ACS Applied Materials & Interfaces 2022, 14 (50) , 56087-56096. https://doi.org/10.1021/acsami.2c16205
    6. Miguel Gonzalez, Krysten Minnici, Bailey Risteen, Lei Wang, Lisa M. Housel, Genesis D. Renderos, Kenneth J. Takeuchi, Esther S. Takeuchi, Amy C. Marschilok, Thomas F. Fuller, Elsa Reichmanis. Active Material Interfacial Chemistry and Its Impact on Composite Magnetite Electrodes. ACS Applied Energy Materials 2021, 4 (9) , 9836-9847. https://doi.org/10.1021/acsaem.1c01882
    7. Hannah F. Mathews, Tolga Çeper, Tobias Speen, Céline Bastard, Selin Bulut, Maria I. Pieper, Felix H. Schacher, Laura De Laporte, Andrij Pich. Engineering poly(dehydroalanine)-based gels via droplet-based microfluidics: from bulk to microspheres. Soft Matter 2024, 20 (31) , 6231-6246. https://doi.org/10.1039/D4SM00676C
    8. Kathrin Kowalczuk, Peter J. Mons, Hans F. Ulrich, Valentin D. Wegner, Johannes C. Brendel, Alexander S. Mosig, Felix H. Schacher. Asymmetric Block Extension of Star‐Shaped [PEG‐SH] 4 – toward Poly(dehydroalanine)‐Functionalized PEG Hydrogels for Catch and Release of Charged Guest Molecules. Macromolecular Bioscience 2024, 24 (2) https://doi.org/10.1002/mabi.202300230
    9. Afshin Nabiyan, Christof Neumann, Andrey Turchanin, Felix H. Schacher. Hybrid nanoreactors formed by interpolyelectrolyte complex formation: a colloidal platform for light-driven catalysis. Journal of Materials Chemistry A 2024, 49 https://doi.org/10.1039/D4TA01824A
    10. Niamh Bayliss, Bernhard V.K.J. Schmidt. Hydrophilic polymers: Current trends and visions for the future. Progress in Polymer Science 2023, 147 , 101753. https://doi.org/10.1016/j.progpolymsci.2023.101753
    11. Ali Zardehi‐Tabriz, Yoones Ghayebzadeh, Amirhossein Enayati Gerdroodbar, Marzieh Golshan, Hossein Roghani‐Mamaqani, Mehdi Salami‐Kalajahi. Polyampholyte Polymers‐Based Sensors: A Review on Stimuli and Applications. Macromolecular Materials and Engineering 2023, 308 (12) https://doi.org/10.1002/mame.202300179
    12. Peter J. Mons, Purushottam Poudel, Marius Hingel, Felix H. Schacher. Synthesis and post-polymerization modification of star-shaped poly(ethylene glycol)- block -polydehydroalanine block copolymers: a versatile template for designing multifunctional polymers. Polymer Chemistry 2023, 14 (31) , 3600-3609. https://doi.org/10.1039/D3PY00622K
    13. Yusuke Sakamoto, Tomoki Nishimura. Recent advances in the self-assembly of sparsely grafted amphiphilic copolymers in aqueous solution. Polymer Chemistry 2022, 13 (46) , 6343-6360. https://doi.org/10.1039/D2PY01018F
    14. Peter J. Mons, Nora Fribiczer, Kathrin Kowalczuk, Purushottam Poudel, Sebastian Seiffert, Felix H. Schacher. Double hydrophilic poly(ethylene glycol)- block -poly(dehydroalanine) four-arm star block copolymers: synthesis and solution behavior. Polymer Chemistry 2022, 13 (29) , 4298-4308. https://doi.org/10.1039/D2PY00579D
    15. Afshin Nabiyan, Johannes Bernhard Max, Christof Neumann, Magdalena Heiland, Andrey Turchanin, Carsten Streb, Felix Helmut Schacher. Polyampholytic Graft Copolymers as Matrix for TiO 2 /Eosin Y/[Mo 3 S 13 ] 2− Hybrid Materials and Light‐Driven Catalysis. Chemistry – A European Journal 2021, 27 (68) , 16924-16929. https://doi.org/10.1002/chem.202100091
    16. Johannes B. Max, Afshin Nabiyan, Jonas Eichhorn, Felix H. Schacher. Triple‐Responsive Polyampholytic Graft Copolymers as Smart Sensors with Varying Output. Macromolecular Rapid Communications 2021, 42 (7) https://doi.org/10.1002/marc.202000671
    17. Daniel Costabel, Artem Skabeev, Afshin Nabiyan, Yusen Luo, Johannes B. Max, Ashwene Rajagopal, Daniel Kowalczyk, Benjamin Dietzek, Maria Wächtler, Helmar Görls, Dirk Ziegenbalg, Yulian Zagranyarski, Carsten Streb, Felix H. Schacher, Kalina Peneva. 1,7,9,10‐Tetrasubstituted PMIs Accessible through Decarboxylative Bromination: Synthesis, Characterization, Photophysical Studies, and Hydrogen Evolution Catalysis. Chemistry – A European Journal 2021, 27 (12) , 4081-4088. https://doi.org/10.1002/chem.202004326
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    Macromolecules

    Cite this: Macromolecules 2020, 53, 11, 4511–4523
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.0c00474
    Published May 20, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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