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Polymer Brush-Functionalized Chitosan Hydrogels as Antifouling Implant Coatings
Implantable 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.
GaN-based radial heterostructure nanowires grown by MBE and ALD
A combination of molecular beam epitaxy (MBE) and atomic layer deposition (ALD) was adopted to fabricate GaN-based core/shell NW structures. ALD was used to deposit a HfO2 shell of onto the MBE grown GaN NWs. Electron transparent samples were prepared by focussed ion beam methods and characterized using state-of-the-art analytical transmission and scanning transmission electron microscopy. The polycrystalline coating was found to be uniform along the whole length of the NWs. Photoluminescence and Raman spectroscopy analysis confirms that the HfO2 ALD coating does not add any structural defect when deposited on the NWs.
Multifunctional coatings combining bioactive peptides and affinity-based cytokine delivery for enhanced integration of degradable vascular grafts
Insufficient endothelialization of cardiovascular devices is a high-risk factor for implant failure. Presentation of extracellular matrix (ECM)-derived coatings is a well-known strategy to improve implant integration. However, the complexity of the system is challenging and strategies for applying multifunctionality are required. Here, we engineered mussel-derived surface-binding peptides equipped with integrin (c[RGDfK]) and proteoglycan binding sites (FHRRIKA) for enhanced endothelialization. Surface-binding properties of the platform containing l-3,4-dihydroxyphenylalanine (DOPA) residues were confirmed for hydrophilized polycaprolactone-co-lactide scaffolds as well as for glass and polystyrene. Further, heparin and the heparin-binding angiogenic factors VEGF, FGF-2 and CXCL12 were immobilized onto the peptide in a modular assembly. Presentation of bioactive peptides greatly enhanced human umbilical vein endothelial cell (HUVEC) adhesion and survival under static and fluidic conditions. In subsequent investigations, peptide-heparin-complexes loaded with CXCL12 or VEGF had an additional increasing effect on cell viability, differentiation and migration. Finally, hemocompatibility of the coatings was ensured. This study demonstrates that coatings combining adhesion peptides, glycosaminoglycans and modulators are a versatile tool to convey ECM-inspired multifunctionality to biomaterials and efficiently promote their integration. © 2020 The Royal Society of Chemistry.
Endothelium-Mimicking Multifunctional Coating Modified Cardiovascular Stents via a Stepwise Metal-Catechol-(Amine) Surface Engineering Strategy
Stenting is currently the major therapeutic treatment for cardiovascular diseases. However, the nonbiogenic metal stents are inclined to trigger a cascade of cellular and molecular events including inflammatory response, thrombogenic reactions, smooth muscle cell hyperproliferation accompanied by the delayed arterial healing, and poor reendothelialization, thus leading to restenosis along with late stent thrombosis. To address prevalence critical problems, we present an endothelium-mimicking coating capable of rapid regeneration of a competently functioning new endothelial layer on stents through a stepwise metal (copper)-catechol-(amine) (MCA) surface chemistry strategy, leading to combinatorial endothelium-like functions with glutathione peroxidase-like catalytic activity and surface heparinization. Apart from the stable nitric oxide (NO) generating rate at the physiological level (2:2 × 10a'10 mol/cm2/min lasting for 60 days), this proposed strategy could also generate abundant amine groups for allowing a high heparin conjugation efficacy up to ∼1 μg/cm2, which is considerably higher than most of the conventional heparinized surfaces. The resultant coating could create an ideal microenvironment for bringing in enhanced antithrombogenicity, anti-inflammation, anti-proliferation of smooth muscle cells, re-endothelialization by regulating relevant gene expressions, hence preventing restenosis in vivo. We envision that the stepwise MCA coating strategy would facilitate the surface endothelium-mimicking engineering of vascular stents and be therefore helpful in the clinic to reduce complications associated with stenosis. © 2020 American Association for the Advancement of Science. All rights reserved.
Double-Hydrophobic-Coating through Quenching for Hydrogels with Strong Resistance to Both Drying and Swelling
In recent years, various hydrogels with a wide range of functionalities have been developed. However, owing to the two major drawbacks of hydrogels—air-drying and water-swelling—hydrogels developed thus far have yet to achieve most of their potential applications. Herein, a bioinspired, facile, and versatile method for fabricating hydrogels with high stability in both air and water is reported. This method includes the creation of a bioinspired homogeneous fusion layer of a hydrophobic polymer and oil in the outermost surface layer of the hydrogel via a double-hydrophobic-coating produced through quenching. As a proof-of-concept, this method is applied to a polyacrylamide hydrogel without compromising its mechanical properties. The coated hydrogel exhibits strong resistance to both drying in air and swelling in multiple aqueous environments. Furthermore, the versatility of this method is demonstrated using different types of hydrogels and oils. Because this method is easy to apply and is not dependent on hydrogel surface chemistry, it can significantly broaden the scope of next-generation hydrogels for real-world applications in both wet and dry environments.
Relevance of interactions between starch-based coatings and plum fruit surfaces: A physical-chemical analysis
In order to extend the shelf life of the fruit, improve appearance, and to keep all nutrition properties of the plum from diminishing, edible coatings comprised of wheat starch and wheat starch–whey protein isolate (in ratio 80/20) were created. Stand-alone films were produced to assess properties which helped to understand the phenomena occurring on the surface level of coated plums. The properties of coatings based on starch are similar to starch coatings containing oil because the natural epicuticular wax layer of plums merges with coating materials. Adding oil doubled the contact angle value and the dispersive component of the surface tension. The workings of adhesion and cohesion, spreading coefficient, water absorption, water content, and solubility in water of the films decreased. Similar processes were observed on the fruits’ surface. In appearance, the coating process is similar to polishing the plum surface for removing crystalline wax. The color parameters of coated fruits did not significantly change. Newly formed bonds or interactions established between starch, whey proteins, water, glycerol, and oil are displayed by Fourier transform infrared (FTIR) analysis. This work revealed how the interactions between the epicuticular wax on the fruit’s surface and the hydrocolloid-based coatings affect the efficiency of the coatings. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
Coating of Carbon Nanotube Fibers: Variation of Tensile Properties, Failure Behavior, and Adhesion Strength
An experimental study of the tensile properties of CNT fibers and their interphasial behavior in epoxy matrices is reported. One of the most promising applications of CNT fibers is their use as reinforcement in multifunctional composites. For this purpose, an increase of the tensile strength of the CNT fibers in unidirectional composites as well as strong interfacial adhesion strength is desirable. However, the mechanical performance of the CNT fiber composites manufactured so far is comparable to that of commercial fiber composites. The interfacial properties of CNT fiber/polymer composites have rarely been investigated and provided CNT fiber/epoxy interfacial shear strength (IFSS) of 14.4 MPa studied by the microbond test. In order to improve the mechanical performance of the CNT fibers, an epoxy compatible coating with nano-dispersed aqueous-based polymeric film formers and low viscous epoxy resin, respectively, was applied. For impregnation of high homogeneity, low molecular weight epoxy film formers and polyurethane film formers were used. The aqueous-based epoxy film formers were not crosslinked and able to interdiffuse with the matrix resin after impregnation. Due to good wetting of the individual CNT fibers by the film formers, the degree of activation of the fibers was improved, leading to increased tensile strength and Young’s modulus. Cyclic tensile loading and simultaneous determination of electric resistance enabled to characterize the fiber’s durability in terms of elastic recovery and hysteresis. The pull-out tests and SEM study reveal different interfacial failure mechanisms in CNT fiber/epoxy systems for untreated and film former treated fibers, on the one hand, and epoxy resin treated ones, on the other hand. The epoxy resin penetrated between the CNT bundles in the reference or film former coated fiber, forming a relatively thick CNT/epoxy composite layer and thus shifting the fracture zone within the fiber. In contrast to this, shear sliding along the interface between the matrix and the outer fiber layer impregnated with the resin was observed for epoxy resin-coated fibers. These fibers have been successfully pulled out of the matrix droplets and shown that the average local interfacial shear stress value was 63 MPa (with apparent IFSS values 33–60 MPa). The interfacial frictional stress between the fiber and the matrix was rather high (9.5 MPa), which can be attributed to the complex structure of the interface and the fiber twisting.
Large-area wet-chemical deposition of nanoporous tungstic silica coatings
We report on a facile procedure for synthesis of nanoporous coatings of tungstic silica through wet-chemical deposition and post-treatment of tungsten-doped potassium silicate solutions. The process relies on an aqueous washing and ion exchange step where dispersed potassium salt deposits are removed from a 150 nm silicate gel layer. Through an adjustment of the pH value of the washing agent within the solubility regime of a tungstic salt precursor, the tungsten content of the remaining nanostructured coating can be controlled. We propose this route as a universal approach for the deposition of large-area coatings of nanoporous silica with the potential for incorporating a broad variety of other dopant species. As for the present case, we observe, on the one hand, antireflective properties which enable the reduction of reflection losses from float glass by up to 3.7 percent points. On the other hand, the incorporation of nanoscale tungstic precipitates provides a lever for tailoring the coating hydrophilicity and, eventually, also surface acidity. This may provide a future route for combining optical performance with anti-fouling functionality.
SPION@polydehydroalanine hybrid particles
It is generally accepted that a protein corona is rapidly formed upon exposure of nanoparticles to biological fluids and that both the amount and the composition of adsorbed proteins affect the dispersion properties of the resulting particles. Hereby, the net charge and overall charge density of the pristine nanoparticles are supposed to play a crucial role. In an attempt to control both charge and charge distribution, we report on the coating of superparamagnetic iron oxide nanoparticles (SPIONs) with different polyelectrolytes. Starting from orthogonally protected polydehydroalanine, the material can be easily transformed into a polyanion (poly(tert-butoxycarbonyl acrylic acid), PtBAA), polycation (poly(aminomethylacrylate), PAMA), or even a polyzwitterion (polydehydroalanine, PDha). While coating of SPIONs with PtBAA and PDha was shown to be successful, approaches using PAMA have failed so far. The dispersion properties of the resulting hybrid particles have been investigated using dynamic light scattering (DLS), zeta-potential, and TEM measurements – the amount of adsorbed polymer was quantified using vibrating sample magnetometry (VSM) and thermogravimetric analysis (TGA).