Keywords: Fragmentation Chain-Transfer ; Self-Assembled Monolayers ; Walled Carbon Nanotubes ; Well-Defined Polymer ; Nitroxide-Mediated Polymerization ; Block-Copolymer Brushes ; Poly(Methyl Methacrylate) Brushes ; Transfer Raft Polymerization ; Quartz-Crystal Microbalance ; Poly(Acrylic Acid) Brushes Reference EPFL-REVIEW-148464doi:10.1021/cr900045aView record in Web of Science Record created on 2010-04-23, modified on 2017-05-10

Polymer Brushes via Surface-Initiated Controlled Radical Polymerization: Synthesis, Characterization, Properties, and Applications

The generation of polymer brushes by surface-initiated controlled radical polymerization (SI-CRP) techniques has become a powerful approach to tailor the chemical and physical properties of interfaces and has given rise to great advances in surface and interface engineering. Polymer brushes are defined as thin polymer films in which the individual polymer chains are tethered by one chain end to a solid interface. Significant advances have been made over the past years in the field of polymer brushes. This includes novel developments in SI-CRP, as well as the emergence of novel applications such as catalysis, electronics, nanomaterial synthesis and biosensing. Additionally, polymer brushes prepared via SI-CRP have been utilized to modify the surface of novel substrates such as natural fibers, polymer nanofibers, mesoporous materials, graphene, viruses and protein nanoparticles. The last years have also seen exciting advances in the chemical and physical characterization of polymer brushes, as well as an ev...

Surface-Initiated Controlled Radical Polymerization: State-of-the-Art, Opportunities, and Challenges in Surface and Interface Engineering with Polymer Brushes

Surface modifications by polymers are becoming increasingly important for various applications ranging from biotechnology to advanced microelectronics. Recent successful applications of living radical polymerization (LRP) made it possible to graft various low-polydispersity polymers including simple homopolymers, end-functionalized polymers, block/random/gradient copolymers, and functional polymers. At the same time, this technique has brought about a striking increase of graft density. Graft chains in such a high-density polymer brush were found to be highly extended in good solvent, even to the order of their full lengths. It was also found that a high-density polymer brush has characteristic properties, in both swollen and dry states, quite different and unpredictable from those of the semi-dilute or moderately dense polymer brushes previously studied. This review highlights the recent development of surface-initiated LRP and the structures, properties, and potential applications of thereby obtainable high-density polymer brushes. It is believed that surface-initiated LRP is opening up a new route to "precision" surface modification.

Structure and properties of high-density polymer brushes prepared by surface-initiated living radical polymerization

Biological membranes play an essential role in living organisms by providing stable and functional compartments, preserving cell architecture, whilst supporting signalling and selective transport that are mediated by a variety of proteins embedded in the membrane. However, mimicking cell membranes – to be applied in artificial systems – is very challenging because of the vast complexity of biological structures. In this respect a highly promising strategy to designing multifunctional hybrid materials/systems is to combine biological molecules with polymer membranes or to design membranes with intrinsic stimuli-responsive properties. Here we present supramolecular polymer assemblies resulting from self-assembly of mostly amphiphilic copolymers either as 3D compartments (polymersomes, PICsomes, peptosomes), or as planar membranes (free-standing films, solid-supported membranes, membrane-mimetic brushes). In a bioinspired strategy, such synthetic assemblies decorated with biomolecules by insertion/encapsulation/attachment, serve for development of multifunctional systems. In addition, when the assemblies are stimuli-responsive, their architecture and properties change in the presence of stimuli, and release a cargo or allow “on demand” a specific in situ reaction. Relevant examples are included for an overview of bioinspired polymer compartments with nanometre sizes and membranes as candidates in applications ranging from drug delivery systems, up to artificial organelles, or active surfaces. Both the advantages of using polymer supramolecular assemblies and their present limitations are included to serve as a basis for future improvements.

/pdf/bioinspired-polymer-vesicles-and-membranes-for-biological-3d546sxrk4.pdf

Bioinspired polymer vesicles and membranes for biological and medical applications

Radical Polymerization and Copper(0) Mediated Polymerization): From Fundamentals to Bioapplications Cyrille Boyer,*,†,‡ Nathaniel Alan Corrigan,‡ Kenward Jung,‡ Diep Nguyen,‡ Thuy-Khanh Nguyen,‡ Nik Nik M. Adnan,†,‡ Susan Oliver,†,‡ Sivaprakash Shanmugam,‡ and Jonathan Yeow†,‡ †Australian Centre for Nanomedicine, and ‡Centre for Advanced Macromolecular Design (CAMD), School of Chemical Engineering, University of New South Wales, Sydney 2052, Australia

Copper-Mediated Living Radical Polymerization (Atom Transfer Radical Polymerization and Copper(0) Mediated Polymerization): From Fundamentals to Bioapplications

Diblock copolymer polyelectrolyte brushes of either polystyrene (PS) or poly(methyl acrylate) (PMA) and poly(acrylic acid) (PAA) were synthesized using sequential monomer addition from a tethered 2...

Synthesis, Characterization, and Properties of Polyelectrolyte Block Copolymer Brushes Prepared by Atom Transfer Radical Polymerization and Their Use in the Synthesis of Metal Nanoparticles

We present an account of our research into polyelectrolyte polymer brushes that are capable of acting as stimuli-responsive films. We first detail the synthesis of poly(acrylic acid) polymer brushes using ATRP in a “grafting from” strategy. Significantly, we employed a chemical-free deprotection step that should leave the anchoring ester groups intact. We have demonstrated how these polymer assemblies respond to stimuli such as pH and electrolyte concentration. We have used poly(acrylic acid) polymer brushes for the synthesis of metallic nanoparticles and review this work. We have used XPS, ATR-FTIR, and AFM spectroscopy to show the presence of silver and palladium nanoparticles within polymer brushes. Finally, we report the synthesis of AB diblock polyampholyte polymer brushes that represent an extension of polyelectrolyte polymer brushes.

Stimuli-Responsive Polyelectrolyte Polymer Brushes Prepared via Atom-Transfer Radical Polymerization†

The surface rearrangement of polymer brushes composed of diblock copolymer chains with fluoropolymer blocks has been shown to be readily induced using thermal annealing. Changes in surface composition accomplished by the rearrangement were demonstrated by tensiometry and atomic force microscopy (AFM). Most of the research focused on brushes consisting of a hydrocarbon inner block [either poly(methyl acrylate) or polystyrene] and a fluoropolymer outer block [poly(pentafluorostyrene), poly(heptadecafluorodecyl acrylate), poly(pentafluoropropyl acrylate), or poly(trifluoroethyl acrylate)]. The diblock copolymer brushes were first treated with a block selective solvent for the hydrocarbon block. Rearrangement was complete for all brushes except those in which poly(heptadecafluorodecyl acrylate) was the outer block. Subsequentially, the surfaces were then thermally treated to allow the fluoropolymer to migrate to the surface. The optimal temperature and exposure time for thermal treatment were found to vary wi...

Thermoresponsive Behavior of Semifluorinated Polymer Brushes

The role that alkyl chain packing density in a self-assembled monolayer (SAM) plays in the adsorption of protein to the SAM surface was investigated using in situ neutron reflectivity (NR) and tota...

Changes in Protein Adsorption on Self-Assembled Monolayers with Monolayer Order: Comparison of Human Serum Albumin and Human Gamma Globulin

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Synthesis, Characterization, and Properties of Polyelectrolyte Block Copolymer Brushes Prepared by Atom Transfer Radical Polymerization and Their Use in the Synthesis of Metal Nanoparticles

Stimuli-Responsive Polyelectrolyte Polymer Brushes Prepared via Atom-Transfer Radical Polymerization†

Thermoresponsive Behavior of Semifluorinated Polymer Brushes

Changes in Protein Adsorption on Self-Assembled Monolayers with Monolayer Order: Comparison of Human Serum Albumin and Human Gamma Globulin