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- ItemPolymer Brush-Functionalized Chitosan Hydrogels as Antifouling Implant Coatings(Columbus, Ohio : American Chemical Society, 2017) Buzzacchera, Irene; Vorobii, Mariia; Kostina, Nina Yu; de Los Santos Pereira, Andres; Riedel, Tomáš; Bruns, Michael; Ogieglo, Wojciech; Möller, Martin; Wilson, Christopher J.; Rodriguez-Emmenegger, CesarImplantable sensor devices require coatings that efficiently interface with the tissue environment to mediate biochemical analysis. In this regard, bioinspired polymer hydrogels offer an attractive and abundant source of coating materials. However, upon implantation these materials generally elicit inflammation and the foreign body reaction as a consequence of protein fouling on their surface and concomitant poor hemocompatibility. In this report we investigate a strategy to endow chitosan hydrogel coatings with antifouling properties by the grafting of polymer brushes in a "grafting-from" approach. Chitosan coatings were functionalized with polymer brushes of oligo(ethylene glycol) methyl ether methacrylate and 2-hydroxyethyl methacrylate using photoinduced single electron transfer living radical polymerization and the surfaces were thoroughly characterized by XPS, AFM, water contact angle goniometry, and in situ ellipsometry. The antifouling properties of these new bioinspired hydrogel-brush coatings were investigated by surface plasmon resonance. The influence of the modifications to the chitosan on hemocompatibility was assessed by contacting the surfaces with platelets and leukocytes. The coatings were hydrophilic and reached a thickness of up to 180 nm within 30 min of polymerization. The functionalization of the surface with polymer brushes significantly reduced the protein fouling and eliminated platelet activation and leukocyte adhesion. This methodology offers a facile route to functionalizing implantable sensor systems with antifouling coatings that improve hemocompatibility and pave the way for enhanced device integration in tissue.
- ItemTEMPO‐Modified Polymethacrylates as Mediators in Electrosynthesis – Redox Behavior and Electrocatalytic Activity toward Alcohol Substrates(Weinheim : Wiley-VCH, 2021) Mohebbati, Nayereh; Prudlik, Adrian; Scherkus, Anton; Gudkova, Aija; Francke, RobertHomogeneous catalysts (“mediators”) are useful for tuning selectivity in organic electrosynthesis. However, they can have a negative impact on the overall mass and energy balance if used only once or recycled inefficiently. In a previous work, we introduced the polymediator concept, in which soluble redox-active polymers catalyze the electrochemical reaction, allowing for recovery by dialysis or pressure-driven membrane filtration. Using anodic alcohol oxidation as a test case, it was shown that TEMPO-modified polymethacrylates (TPMA) can serve as efficient and reusable mediators. In the present study, the properties of a TPMA sample with well-defined molecular weight distribution were studied using cyclic voltammetry and compared to low-molecular TEMPO species. The non-catalytic profiles of TPMA are shaped by diffusive and adsorptive processes, whereby the latter only become pronounced at low mediator concentrations and high scan rates. Electrocatalytic studies suggest that under the applied conditions, TPMA-catalyzed alcohol oxidation is a predominantly homogeneous process. The homogeneous kinetics are determined rather by the mediator potential than by steric influences of the polymer backbone. © 2021 The Authors. ChemElectroChem published by Wiley-VCH GmbH
- ItemSemi-Interpenetrating Polymer Networks Based on N-isopropylacrylamide and 2-acrylamido-2-methylpropane Sulfonic Acid for Intramolecular Force-Compensated Sensors(Bristol : IOP Publishing, 2021) Binder, Simon; Zschoche, Stefan; Voit, Brigitte; Gerlach, GeraldStimulus-responsive hydrogels are swellable polymers that take up a specific volume depending on a measured variable present in solution. Hydrogel-based chemical sensors make use of this ability by converting the resulting swelling pressure, which depends on the measured variable, into an electrical value. Due to the tedious swelling processes, the measuring method of intramolecular force compensation is used to suppress these swelling processes and, thus, significantly increase the sensor's response time. However, intramolecular force compensation requires a bisensitive hydrogel. In addition to the sensitivity of the measured variable the gel has to provide a second sensitivity for intrinsic compensation of the swelling pressure. At the same time, this hydrogel has to meet further requirements, e.g. high compressive strength. Until now, interpenetrating polymer networks (IPN) have been used for such a force-compensatory effective hydrogel, which are complex to manufacture. In order to significantly simplify the sensor design and production, a simpler synthesis of the bisensitive hydrogel is desirable. This paper presents a new bisensitive hydrogel based on semi-interpenetrating polymer networks. It is based on a copolymer network consisting of N-isopropylacrylamide (NiPAAm) and 2-acrylamido-2-methylpropane sulfonic acid (AMPS) and long PAMPS strands that permeate it. Measurements show, that this hydrogel meets all essential requirements for intramolecular force compensation and is at the same time much easier to synthesize than previously used IPN hydrogels. © 2021 The Author(s).
- ItemSingle-Polymer Friction Force Microscopy of dsDNA Interacting with a Nanoporous Membrane(Washington, DC : ACS Publ., 2023) Schellnhuber, Kordula; Blass, Johanna; Hübner, Hanna; Gallei, Markus; Bennewitz, RolandSurface-grafted polymers can reduce friction between solids in liquids by compensating the normal load with osmotic pressure, but they can also contribute to friction when fluctuating polymers entangle with the sliding counter face. We have measured forces acting on a single fluctuating double-stranded DNA polymer, which is attached to the tip of an atomic force microscope and interacts intermittently with nanometer-scale methylated pores of a self-assembled polystyrene-block-poly(4-vinylpyridine) membrane. Rare binding of the polymer into the pores is followed by a stretching of the polymer between the laterally moving tip and the surface and by a force-induced detachment. We present results for the velocity dependence of detachment forces and of attachment frequency and discuss them in terms of rare excursions of the polymer beyond its equilibrium configuration.
- ItemExploring the colloid-to-polymer transition for ultra-low crosslinked microgels from three to two dimensions([London] : Nature Publishing Group UK, 2019) Scotti, A.; Bochenek, S.; Brugnoni, M.; Fernandez-Rodriguez, M.A.; Schulte, M.F.; Houston, J.E.; Gelissen, A.P.H.; Potemkin, I.I.; Isa, L.; Richtering, W.Microgels are solvent-swollen nano- and microparticles that show prevalent colloidal-like behavior despite their polymeric nature. Here we study ultra-low crosslinked poly(N-isopropylacrylamide) microgels (ULC), which can behave like colloids or flexible polymers depending on dimensionality, compression or other external stimuli. Small-angle neutron scattering shows that the structure of the ULC microgels in bulk aqueous solution is characterized by a density profile that decays smoothly from the center to a fuzzy surface. Their phase behavior and rheological properties are those of soft colloids. However, when these microgels are confined at an oil-water interface, their behavior resembles that of flexible macromolecules. Once monolayers of ultra-low crosslinked microgels are compressed, deposited on solid substrate and studied with atomic-force microscopy, a concentration-dependent topography is observed. Depending on the compression, these microgels can behave as flexible polymers, covering the substrate with a uniform film, or as colloidal microgels leading to a monolayer of particles.
- ItemHomopolymerization of ethylene, 1-hexene, styrene and copolymerization of styrene with 1,3-cyclohexadiene using (η5- tetramethylcyclopentadienyl)dimethylsilyl(N-Ar')amido-TiCl2/MAO (Ar'=6-(2-(diethylboryl)phenyl)pyrid-2-yl, biphen-3-yl)(Basel : MDPI AG, 2011) Camadanli, S.; Decker, U.; Kühnel, C.; Reinhardt, I.; Buchmeiser, M.R.The propensity of a half-sandwich (η55- tetramethylcyclopentadienyl) dimethylsilylamido TiIV-based catalyst bearing an auxiliary diethylboryl-protected pyridyl moiety (Ti-8), activated by methylaluminoxane (MAO) to homopolymerize α-olefins such as ethylene, 1-hexene and styrene as well as to copolymerize styrene with 1,3-cyclohexadiene is described. The reactivity of Ti-8 was investigated in comparison to a 6-(2-(diethylboryl)phenyl)pyrid-2-yl-free analogue (Ti-3).
- ItemSimultaneous Treatment of Both Sides of the Polymer with a Conical-Shaped Atmospheric Pressure Plasma Jet(Basel : MDPI, 2023) Kodaira, Felipe Vicente de Paula; Leal, Bruno Henrique Silva; Tavares, Thayna Fernandes; Quade, Antje; Hein, Luis Rogerio de Oliveira; Chiappim, William; Kostov, Konstantin GeorgievA conical-shaped atmospheric pressure plasma jet (CS-APPJ) was developed to overcome a standard limitation of APPJs, which is their small treatment area. The CS-APPJs increase the treatment area but use the same gas flow. In the present work, polypropylene samples were treated by CS-APPJ and characterized by scanning electron microscope (SEM), the contact angle, Fourier-transformed infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). It was observed that the treatment co-occurs on the face directly in contact with the plasma and on the opposite face (OF) of the samples, i.e., no contact. However, the treatment changed the chemical composition on each side; the OF is rougher than the direct contact face (DCF), probably due to the oxygen groups in excess at the DCF and nitrogen in quantity at the OF. Although simultaneous treatment of both sides of the sample occurs for most atmospheric plasma treatments, this phenomenon is not explored in the literature.
- ItemSimultaneous Treatment of Both Sides of the Polymer with a Conical-Shaped Atmospheric Pressure Plasma Jet(Basel : MDPI, 2023) Kodaira, Felipe Vicente de Paula; Leal, Bruno Henrique Silva; Tavares, Thayna Fernandes; Quade, Antje; Hein, Luis Rogerio de Oliveira; Chiappim, William; Kostov, Konstantin GeorgievA conical-shaped atmospheric pressure plasma jet (CS-APPJ) was developed to overcome a standard limitation of APPJs, which is their small treatment area. The CS-APPJs increase the treatment area but use the same gas flow. In the present work, polypropylene samples were treated by CS-APPJ and characterized by scanning electron microscope (SEM), the contact angle, Fourier-transformed infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). It was observed that the treatment co-occurs on the face directly in contact with the plasma and on the opposite face (OF) of the samples, i.e., no contact. However, the treatment changed the chemical composition on each side; the OF is rougher than the direct contact face (DCF), probably due to the oxygen groups in excess at the DCF and nitrogen in quantity at the OF. Although simultaneous treatment of both sides of the sample occurs for most atmospheric plasma treatments, this phenomenon is not explored in the literature.