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Dispersity within Brushes Plays a Major Role in Determining Their Interfacial Properties: The Case of Oligoxazoline-Based Graft Polymers.
Romio, Matteo; Grob, Benjamin; Trachsel, Lucca; Mattarei, Andrea; Morgese, Giulia; Ramakrishna, Shivaprakash N; Niccolai, Francesca; Guazzelli, Elisa; Paradisi, Cristina; Martinelli, Elisa; Spencer, Nicholas D; Benetti, Edmondo M.
Afiliación
  • Romio M; Biointerfaces Lab, Swiss Federal Laboratories for Materials Science and Technology (Empa), Lerchenfeldstrasse 5, 9014 St. Gallen, Switzerland.
  • Grob B; Laboratory for Surface Science and Technology, Department of Materials, ETH Zürich, Vladimir-Prelog-Weg 5, 8093 Zürich, Switzerland.
  • Trachsel L; Laboratory for Surface Science and Technology, Department of Materials, ETH Zürich, Vladimir-Prelog-Weg 5, 8093 Zürich, Switzerland.
  • Mattarei A; George & Josephine Butler Polymer Research Laboratory, Department of Chemistry, University of Florida, P.O. Box 117200, Gainesville, Florida 32611-7200, United States.
  • Morgese G; Department of Pharmaceutical and Pharmacological Sciences, University of Padova, Via Marzolo 5, 35131 Padova, Italy.
  • Ramakrishna SN; Institute of Materials and Process Engineering (IMPE), School of Engineering (SoE), Zürich University of Applied Sciences (ZHAW), Technikumstrasse 9, 8401 Winterthur, Switzerland.
  • Niccolai F; Soft Materials and Interfaces, Department of Materials, ETH Zürich, Vladimir-Prelog-Weg 5, 8093 Zürich, Switzerland.
  • Guazzelli E; Department of Chemistry and Industrial Chemistry, University of Pisa, Via Moruzzi 13, 56124 Pisa, Italy.
  • Paradisi C; Department of Chemistry and Industrial Chemistry, University of Pisa, Via Moruzzi 13, 56124 Pisa, Italy.
  • Martinelli E; Department of Chemical Sciences, University of Padova, Via Marzolo 1, 35122 Padova, Italy.
  • Spencer ND; Department of Chemistry and Industrial Chemistry, University of Pisa, Via Moruzzi 13, 56124 Pisa, Italy.
  • Benetti EM; Laboratory for Surface Science and Technology, Department of Materials, ETH Zürich, Vladimir-Prelog-Weg 5, 8093 Zürich, Switzerland.
J Am Chem Soc ; 143(45): 19067-19077, 2021 11 17.
Article en En | MEDLINE | ID: mdl-34738797
Many synthetic polymers used to form polymer-brush films feature a main backbone with functional, oligomeric side chains. While the structure of such graft polymers mimics biomacromolecules to an extent, it lacks the monodispersity and structural purity present in nature. Here we demonstrate that side-chain heterogeneity within graft polymers significantly influences hydration and the occurrence of hydrophobic interactions in the subsequently formed brushes and consequently impacts fundamental interfacial properties. This is demonstrated for the case of poly(methacrylate)s (PMAs) presenting oligomeric side chains of different length (n) and dispersity. A precise tuning of brush structure was achieved by first synthesizing oligo(2-ethyl-2-oxazoline) methacrylates (OEOXMAs) by cationic ring-opening polymerization (CROP), subsequently purifying them into discrete macromonomers with distinct values of n by column chromatography, and finally obtaining poly[oligo(2-ethyl-2-oxazoline) methacrylate]s (POEOXMAs) by reversible addition-fragmentation chain-transfer (RAFT) polymerization. Assembly of POEOXMA on Au surfaces yielded graft polymer brushes with different side-chain dispersities and lengths, whose properties were thoroughly investigated by a combination of variable angle spectroscopic ellipsometry (VASE), quartz crystal microbalance with dissipation (QCMD), and atomic force microscopy (AFM) methods. Side-chain dispersity, or dispersity within brushes, leads to assemblies that are more hydrated, less adhesive, and more lubricious and biopassive compared to analogous films obtained from graft polymers characterized by a homogeneous structure.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: Suiza Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: Suiza Pais de publicación: Estados Unidos