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- ItemFibroblast Response to Nanocolumnar TiO2 Structures Grown by Oblique Angle Sputter Deposition(Weinheim : Wiley-VCH, 2021) Kapprell, Uta; Friebe, Sabrina; Grüner, Susann; Grüner, Christoph; Kupferer, Astrid; Rauschenbach, Bernd; Mayr, Stefan G.Cells are established to sense and respond to the properties, including nano- and microscale morphology, of the substrate they adhere to, which opens up the possibility to tailor bioactivity. With this background, the potential of tilted TiO2 nanostructures grown by oblique angle sputtering to affect fibroblasts with particular focus on inducing anisotropy in cell behavior is explored. By depositing TiO2 at different oblique angles relative to the substrate normal, morphologies, columnar tilt angle, roughness, and distances between neighbored nanocolumns can be adjusted. To assess bioactivity of the resulting structures, L929-mouse fibroblasts are seeded in vitro on TiO2 nanostructured substrates. Angle-dependent movement and velocity distributions of the cells on differently tilted columns and a smooth reference sample are studied. Cell proliferation rates and cell areas are additional factors which provide information about viability and the well-being of cells. It could be shown that the local topography of the surface has an influence on the directed movement of the cells. © 2021 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
- ItemMagnetically responsive composites: electron beam assisted magnetic nanoparticle arrest in gelatin hydrogels for bioactuation(Cambridge : RSC Publ., 2019) Deuflhard, Marie; Eberbeck, Dietmar; Hietschold, Philine; Wilharm, Nils; Mühlberger, Marina; Friedrich, Ralf P.; Alexiou, Christoph; Mayr, Stefan G.As emerging responsive materials, ferrogels have become highly attractive for biomedical and technical applications in terms of soft actuation, tissue engineering or controlled drug release. In the present study, bioderived ferrogels were fabricated and successfully deformed within moderate, heterogeneous magnetic fields. Synthesis was realized by arresting iron oxide nanoparticles in porcine gelatin by introduction of covalent crosslinks via treatment with energetic electrons for mesh refinement. This approach also allows for tuning thermal and mechanical stability of the gelatin matrix. Operating the bioferrogel in compression, magnetic forces on the nanoparticles are counterbalanced by the stiffness of the hydrogel matrix that is governed by a shift in thermodynamic equilibrium of swelling, as derived in the framework of osmosis. As gelatin and iron oxide nanoparticles are established as biocompatible constituents, these findings promise potential for in vivo use as contactless mechanical transducers.
- ItemEmploying Nanostructured Scaffolds to Investigate the Mechanical Properties of Adult Mammalian Retinae Under Tension(Basel : Molecular Diversity Preservation International, 2020) Juncheed, Kantida; Kohlstrunk, Bernd; Friebe, Sabrina; Dallacasagrande, Valentina; Maurer, Patric; Reichenbach, Andreas; Mayr, Stefan G.; Zink, MareikeNumerous eye diseases are linked to biomechanical dysfunction of the retina. However, the underlying forces are almost impossible to quantify experimentally. Here, we show how biomechanical properties of adult neuronal tissues such as porcine retinae can be investigated under tension in a home-built tissue stretcher composed of nanostructured TiO2 scaffolds coupled to a self-designed force sensor. The employed TiO2 nanotube scaffolds allow for organotypic long-term preservation of adult tissues ex vivo and support strong tissue adhesion without the application of glues, a prerequisite for tissue investigations under tension. In combination with finite element calculations we found that the deformation behavior is highly dependent on the displacement rate which results in Young’s moduli of (760–1270) Pa. Image analysis revealed that the elastic regime is characterized by a reversible shear deformation of retinal layers. For larger deformations, tissue destruction and sliding of retinal layers occurred with an equilibration between slip and stick at the interface of ruptured layers, resulting in a constant force during stretching. Since our study demonstrates how porcine eyes collected from slaughterhouses can be employed for ex vivo experiments, our study also offers new perspectives to investigate tissue biomechanics without excessive animal experiments. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemCarbon and Neon Ion Bombardment Induced Smoothing and Surface Relaxation of Titania Nanotubes(Basel : MDPI, 2021) Kupferer, Astrid; Mensing, Michael; Lehnert, Jan; Mändl, Stephan; Mayr, Stefan G.Titania nanotube arrays with their enormous surface area are the subject of much attention in diverse fields of research. In the present work, we show that not only 60 keV and 150 keV ion bombardment of amorphous titania nanotube arrays yields defect creation within the tube walls, but it also changes the surface morphology: the surface relaxes and smoothens in accordance with a curvature-driven surface material’s transport mechanism, which is mediated by radiation-induced viscous flow or radiation-enhanced surface diffusion, while the nanotubes act as additional sinks for the particle surface currents. These effects occur independently of the ion species: both carbon and neon ion bombardments result in comparable surface relaxation responses initiated by an ion energy of 60 keV at a fluence of 1 × 1016 ions/cm2. Using atomic force microscopy and contact angle measurements, we thoroughly study the relaxation effects on the surface topography and surface free energy, respectively. Moreover, surface relaxation is accompanied by further amorphization in surface-near regions and a reduction in the mass density, as demonstrated by Raman spectroscopy and X-ray reflectivity. Since ion bombardment can be performed on global and local scales, it constitutes a versatile tool to achieve well-defined and tunable topographies and distinct surface characteristics. Hence, different types of nanotube arrays can be modified for various applications.
- ItemCompositional Patterning in Carbon Implanted Titania Nanotubes(Weinheim : Wiley-VCH, 2021) Kupferer, Astrid; Holm, Alexander; Lotnyk, Andriy; Mändl, Stephan; Mayr, Stefan G.Ranging from novel solar cells to smart biosensors, titania nanotube arrays constitute a highly functional material for various applications. A promising route to modify material characteristics while preserving the amorphous nanotube structure is present when applying low-energy ion implantation. In this study, the interplay of phenomenological effects observed upon implantation of low fluences in the unique 3D structure is reported: sputtering versus readsorption and plastic flow, amorphization versus crystallization and compositional patterning. Patterning within the oxygen and carbon subsystem is revealed using transmission electron microscopy. By applying a Cahn–Hilliard approach within the framework of driven alloys, characteristic length scales are derived and it is demonstrated that compositional patterning is expected on free enthalpy grounds, as predicted by density functional theory based ab initio calculations. Hence, an attractive material with increased conductivity for advanced devices is provided. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemA study on the material properties of novel PEGDA/gelatin hybrid hydrogels polymerized by electron beam irradiation(Lausanne : Frontiers Media, 2023) Şener Raman, Tuğçe; Kuehnert, Mathias; Daikos, Olesya; Scherzer, Tom; Krömmelbein, Catharina; Mayr, Stefan G.; Abel, Bernd; Schulze, AgnesGelatin-based hydrogels are highly desirable biomaterials for use in wound dressing, drug delivery, and extracellular matrix components due to their biocompatibility and biodegradability. However, insufficient and uncontrollable mechanical properties and degradation are the major obstacles to their application in medical materials. Herein, we present a simple but efficient strategy for a novel hydrogel by incorporating the synthetic hydrogel monomer polyethylene glycol diacrylate (PEGDA, offering high mechanical stability) into a biological hydrogel compound (gelatin) to provide stable mechanical properties and biocompatibility at the resulting hybrid hydrogel. In the present work, PEGDA/gelatin hybrid hydrogels were prepared by electron irradiation as a reagent-free crosslinking technology and without using chemical crosslinkers, which carry the risk of releasing toxic byproducts into the material. The viscoelasticity, swelling behavior, thermal stability, and molecular structure of synthesized hybrid hydrogels of different compound ratios and irradiation doses were investigated. Compared with the pure gelatin hydrogel, 21/9 wt./wt. % PEGDA/gelatin hydrogels at 6 kGy exhibited approximately up to 1078% higher storage modulus than a pure gelatin hydrogel, and furthermore, it turned out that the mechanical stability increased with increasing irradiation dose. The chemical structure of the hybrid hydrogels was analyzed by Fourier-transform infrared (FTIR) spectroscopy, and it was confirmed that both compounds, PEGDA and gelatin, were equally present. Scanning electron microscopy images of the samples showed fracture patterns that confirmed the findings of viscoelasticity increasing with gelatin concentration. Infrared microspectroscopy images showed that gelatin and PEGDA polymer fractions were homogeneously mixed and a uniform hybrid material was obtained after electron beam synthesis. In short, this study demonstrates that both the presence of PEGDA improved the material properties of PEGDA/gelatin hybrid hydrogels and the resulting properties are fine-tuned by varying the irradiation dose and PEGDA/gelatin concentration.
- ItemMultifunctional coatings combining bioactive peptides and affinity-based cytokine delivery for enhanced integration of degradable vascular grafts(Cambridge : Royal Soc. of Chemistry, 2020) Clauder, Franziska; Zitzmann, Franziska D.; Friebe, Sabrina; Mayr, Stefan G.; Robitzki, Andrea A.; Beck-Sickinger, Annette G.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.
- ItemLaminin Adsorption and Adhesion of Neurons and Glial Cells on Carbon Implanted Titania Nanotube Scaffolds for Neural Implant Applications(Basel : MDPI, 2022) Frenzel, Jan; Kupferer, Astrid; Zink, Mareike; Mayr, Stefan G.Interfacing neurons persistently to conductive matter constitutes one of the key challenges when designing brain-machine interfaces such as neuroelectrodes or retinal implants. Novel materials approaches that prevent occurrence of loss of long-term adhesion, rejection reactions, and glial scarring are highly desirable. Ion doped titania nanotube scaffolds are a promising material to fulfill all these requirements while revealing sufficient electrical conductivity, and are scrutinized in the present study regarding their neuron–material interface. Adsorption of laminin, an essential extracellular matrix protein of the brain, is comprehensively analyzed. The implantation-dependent decline in laminin adsorption is revealed by employing surface characteristics such as nanotube diameter, (Formula presented.) -potential, and surface free energy. Moreover, the viability of U87-MG glial cells and SH-SY5Y neurons after one and four days are investigated, as well as the material’s cytotoxicity. The higher conductivity related to carbon implantation does not affect the viability of neurons, although it impedes glial cell proliferation. This gives rise to novel titania nanotube based implant materials with long-term stability, and could reduce undesirable glial scarring.
- ItemStructural Breakdown of Collagen Type I Elastin Blend Polymerization(Basel : MDPI, 2022) Wilharm, Nils; Fischer, Tony; Hayn, Alexander; Mayr, Stefan G.Biopolymer blends are advantageous materials with novel properties that may show performances way beyond their individual constituents. Collagen elastin hybrid gels are a new representative of such materials as they employ elastin’s thermo switching behavior in the physiological temperature regime. Although recent studies highlight the potential applications of such systems, little is known about the interaction of collagen and elastin fibers during polymerization. In fact, the final network structure is predetermined in the early and mostly arbitrary association of the fibers. We investigated type I collagen polymerized with bovine neck ligament elastin with up to 33.3 weight percent elastin and showed, by using a plate reader, zeta potential and laser scanning microscopy (LSM) experiments, that elastin fibers bind in a lateral manner to collagen fibers. Our plate reader experiments revealed an elastin concentration-dependent increase in the polymerization rate, although the rate increase was greatest at intermediate elastin concentrations. As elastin does not significantly change the structural metrics pore size, fiber thickness or 2D anisotropy of the final gel, we are confident to conclude that elastin is incorporated homogeneously into the collagen fibers.
- ItemPrograming stimuli-responsiveness of gelatin with electron beams: Basic effects and development of a hydration-controlled biocompatible demonstrator(London : Nature Publishing Group, 2017) Riedel, Stefanie; Heyart, Benedikt; Apel, Katharina S.; Mayr, Stefan G.Biomimetic materials with programmable stimuli responsiveness constitute a highly attractive material class for building bioactuators, sensors and active control elements in future biomedical applications. With this background, we demonstrate how energetic electron beams can be utilized to construct tailored stimuli responsive actuators for biomedical applications. Composed of collagen-derived gelatin, they reveal a mechanical response to hydration and changes in pH-value and ion concentration, while maintaining their excellent biocompatibility and biodegradability. While this is explicitly demonstrated by systematic characterizing an electron-beam synthesized gelatin-based actuator of cantilever geometry, the underlying materials processes are also discussed, based on the fundamental physical and chemical principles. When applied within classical electron beam lithography systems, these findings pave the way for a novel class of highly versatile integrated bioactuators from micro-to macroscales.