Browsing by Author "Mayr, Stefan G."
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- 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.
- ItemCollagen-iron oxide nanoparticle based ferrogel: Large reversible magnetostrains with potential for bioactuation(Bristol : IOP Publishing, 2020) Jauch, Philine; Weidner, Andreas; Riedel, Stefanie; Wilharm, Nils; Dutz, Silvio; Mayr, Stefan G.Smart materials such as stimuli responsive polymeric hydrogels offer unique possibilities for tissue engineering and regenerative medicine. As, however, most synthetic polymer systems and their degradation products lack complete biocompatibility and biodegradability, this study aims to synthesize a highly magnetic responsive hydrogel, based on the abundant natural biopolymer collagen. As the main component of vertebratal extracellular matrix, it reveals excellent biocompatibility. In combination with incorporated magnetic iron oxide nanoparticles, a novel smart nano-bio-ferrogel can be designed. While retaining its basic biophysical properties and interaction with living cells, this collagen-nanoparticle hydrogel can be compressed to 38% of its original size and recovers to 95% in suitable magnetic fields. Besides the phenomenology of this scenario, the underlying physical scenarios are also discussed within the framework of network models. The observed reversible peak strains as large as 150% open up possibilities for the fields of biomedical actuation, soft robotics and beyond. © 2020 The Author(s). Published by IOP Publishing Ltd
- 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
- ItemDesign of biomimetic collagen matrices by reagent-free electron beam induced crosslinking: Structure-property relationships and cellular response(Amsterdam [u.a.] : Elsevier Science, 2019) Riedel, Stefanie; Hietschold, Philine; Krömmelbein, Catharina; Kunschmann, Tom; Konieczny, Robert; Knolle, Wolfgang; Mierke, Claudia T.; Zink, Mareike; Mayr, Stefan G.Novel strategies to mimic mammalian extracellular matrix (ECM) in vitro are desirable to study cell behavior, diseases and new agents in drug delivery. Even though collagen represents the major constituent of mammalian ECM, artificial collagen hydrogels with characteristic tissue properties such as network size and stiffness are difficult to design without application of chemicals which might be even cytotoxic. In our study we investigate how high energy electron induced crosslinking can be utilized to precisely tune collagen properties for ECM model systems. Constituting a minimally invasive approach, collagen residues remain intact in the course of high energy electron treatment. Quantification of the 3D pore size of the collagen network as a function of irradiation dose shows an increase in density leading to decreased pore size. Rheological measurements indicate elevated storage and loss moduli correlating with an increase in crosslinking density. In addition, cell tests show well maintained viability of NIH 3T3 cells for irradiated collagen gels indicating excellent cellular acceptance. With this, our investigations demonstrate that electron beam crosslinked collagen matrices have a high potential as precisely tunable ECM-mimetic systems with excellent cytocompatibility.
- 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.
- ItemEnergetic electron assisted synthesis of highly tunable temperature-responsive collagen/elastin gels for cyclic actuation: macroscopic switching and molecular origins([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Wilharm, Nils; Fischer, Tony; Ott, Florian; Konieczny, Robert; Zink, Mareike; Beck-Sickinger, Annette G.; Mayr, Stefan G.Thermoresponsive bio-only gels that yield sufficiently large strokes reversibly and without large hysteresis at a well-defined temperature in the physiological range, promise to be of value in biomedical application. Within the present work we demonstrate that electron beam modification of a blend of natural collagen and elastin gels is a route to achieve this goal, viz. to synthesize a bioresorbable gel with largely reversible volume contractions as large as 90% upon traversing a transition temperature that can be preadjusted between 36 °C and 43 °C by the applied electron dose. Employing circular dichroism and temperature depending confocal laser scanning microscopy measurements, we furthermore unravel the mechanisms underlying this macroscopic behavior on a molecular and network level, respectively and suggest a stringent picture to account for the experimental observations. © 2019, The Author(s).
- 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
- 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.
- ItemMagnetic measurement methods to probe nanoparticle–matrix interactions(Berlin : de Gruyter, 2021) Liebl, Maik; Eberbeck, Dietmar; Coene, Annelies; Leliaert, Jonathan; Jauch, Philine; Kruteva, Margarita; Fruhner, Lisa; Barnsley, Lester; Mayr, Stefan G.; Wiekhorst, FrankMagnetic nanoparticles (MNPs) are key elements in several biomedical applications, e.g., in cancer therapy. Here, the MNPs are remotely manipulated by magnetic fields from outside the body to deliver drugs or generate heat in tumor tissue. The efficiency and success of these approaches strongly depend on the spatial distribution and quantity of MNPs inside a body and interactions of the particles with the biological matrix. These include dynamic processes of the MNPs in the organism such as binding kinetics, cellular uptake, passage through cell barriers, heat induction and flow. While magnetic measurement methods have been applied so far to resolve the location and quantity of MNPs for therapy monitoring, these methods can be advanced to additionally access these particle–matrix interactions. By this, the MNPs can further be utilized as probes for the physical properties of their molecular environment. In this review, we first investigate the impact of nanoparticle–matrix interactions on magnetic measurements in selected experiments. With these results, we then advanced the imaging modalities magnetorelaxometry imaging and magnetic microsphere tracking to spatially resolve particle–matrix interactions.
- 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.
- ItemMechanical spectroscopy of retina explants at the protein level employing nanostructured scaffolds(London : Royal Soc. of Chemistry, 2016) Rahman, S. Mayazur; Reichenbach, Andreas; Zink, Mareike; Mayr, Stefan G.Development of neuronal tissue, such as folding of the brain, and formation of the fovea centralis in the human retina are intimately connected with the mechanical properties of the underlying cells and the extracellular matrix. In particular for neuronal tissue as complex as the vertebrate retina, mechanical properties are still a matter of debate due to their relation to numerous diseases as well as surgery, where the tension of the retina can result in tissue detachment during cutting. However, measuring the elasticity of adult retina wholemounts is difficult and until now only the mechanical properties at the surface have been characterized with micrometer resolution. Many processes, however, such as pathological changes prone to cause tissue rupture and detachment, respectively, are reflected in variations of retina elasticity at smaller length scales at the protein level. In the present work we demonstrate that freely oscillating cantilevers composed of nanostructured TiO2 scaffolds can be employed to study the frequency-dependent mechanical response of adult mammalian retina explants at the nanoscale. Constituting highly versatile scaffolds with strong tissue attachment for long-term organotypic culture atop, these scaffolds perform damped vibrations as fingerprints of the mechanical tissue properties that are derived using finite element calculations. Since the tissue adheres to the nanostructures via constitutive proteins on the photoreceptor side of the retina, the latter are stretched and compressed during vibration of the underlying scaffold. Probing mechanical response of individual proteins within the tissue, the proposed mechanical spectroscopy approach opens the way for studying tissue mechanics, diseases and the effect of drugs at the protein level.
- 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.
- ItemNanoporous Morphogenesis in Amorphous Carbon Layers: Experiments and Modeling on Energetic Ion Induced Self‐Organization(Weinheim : Wiley-VCH Verlag, 2021) Hoffmann, Daniel T.; Dietrich, Johannes; Mändl, Stephan; Zink, Mareike; Mayr, Stefan G.Nanoporous amorphous carbon constitutes a highly relevant material for a multitude of applications ranging from energy to environmental and biomedical systems. In the present work, it is demonstrated experimentally how energetic ions can be utilized to tailor porosity of thin sputter deposited amorphous carbon films. The physical mechanisms underlying self-organized nanoporous morphogenesis are unraveled by employing extensive molecular dynamics and phase field models across different length scales. It is demonstrated that pore formation is a defect induced phenomenon, in which vacancies cluster in a spinodal decomposition type of self-organization process, while interstitials are absorbed by the amorphous matrix, leading to additional volume increase and radiation induced viscous flow. The proposed modeling framework is capable to reproduce and predict the experimental observations from first principles and thus opens the venue for computer assisted design of nanoporous frameworks.
- 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.
- ItemRegeneration of TiO 2 Nanotube Arrays after Long-Term Cell and Tissue Culture for Multiple Use - An Environmental Scanning Electron Microscopy (ESEM) Survey of Adult Pig Retina and beyond(New York, NY : Springer, 2019) Friebe, Sabrina; Mayr, Stefan G.Long-term organotypic culture of adult tissues not only open up possibilities for studying complex structures of explants in vitro, but also can be employed e.g. to investigate pathological changes, their fingerprints on tissue mechanics, as well as the effectiveness of drugs. While conventional culture methods do not allow for survival times of more than a few days, we have demonstrated recently that TiO 2 nanotube arrays allow to maintain integrity of numerous tissues, including retina, brain, spline and tonsils, for as long as 2 weeks in vitro. A mystery in culturing has been the interaction of tissue with these substrates, which is also reflected by tissue debris after liftoff. As the latter reveals fingerprints of tissue adhesion and impedes with nanotube array reuse, we address within the present environmental scanning electron study debris nature and the effectiveness of cleaning approaches of distinct physical and chemical methods, including UV-light irradiation, O2 plasma treatment and application of an enzyme-based buffer. This will lays the foundation for large-scale regeneration and reuse of nanotube arrays in science and clinical research. © 2019 The Author(s).
- 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.
- 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.
- ItemTailoring morphology in titania nanotube arrays by implantation: experiments and modelling on designed pore size—and beyond(London [u.a.] : Taylor & Francis, 2021) Kupferer, Astrid; Mändl, Stephan; Mayr, Stefan G.Titania nanotube arrays are an exceptionally adaptable material for various applications ranging from energy conversion to biomedicine. Besides electronic properties, structural morphology on nanometre scale is essential. It is demonstrated that ion implantation constitutes a versatile method for the synthesis of tailored nanotube morphologies. Experimental-phenomenological observations reveal a successive closing behaviour of nanotubes upon ion implantation. Employing molecular dynamics calculations in combination with analytical continuum models, the physical origins of this scenario are unravelled by identifying ion bombardment induced viscous flow driven by capillarity as its underlying mechanism besides minor contributions from sputtering and redeposition. These findings enable the tailoring of nanotube arrays suitable for manifold applications.
- ItemThermal and structural properties of the martensitic transformations in Fe7Pd3 shape memory alloys: An ab initio-based molecular dynamics study([London] : IOP, 2019) Holm, Alexander; Mayr, Stefan G.Ferromagnetic shape memory alloys, including the Fe7Pd3 system, constitute an upcoming class of functional materials, whose atomic-scale physical foundations are still insufficiently understood. The present work employs molecular dynamics simulations, based on ab initio derived embedded atom method potentials, to study martensitic transformations and twin variant reorientation. We address thermal and stress induced austenite-martensite transitions, twinning, as well as twin boundary mobility. While the predicted thermal properties are in accordance with experimental observations, we explore the detailed crystallography underlying transformation as well as twin boundary motion. © 2019 The Author(s).
- ItemA Versatile Macromer-Based Glycosaminoglycan (sHA3) Decorated Biomaterial for Pro-Osteogenic Scavenging of Wnt Antagonists(Basel : MDPI, 2020) Gronbach, Mathis; Mitrach, Franziska; Möller, Stephanie; Rother, Sandra; Friebe, Sabrina; Mayr, Stefan G.; Schnabelrauch, Matthias; Hintze, Vera; Hacker, Michael C.; Schulz-Siegmund, MichaelaHigh serum levels of Wnt antagonists are known to be involved in delayed bone defect healing. Pharmaceutically active implant materials that can modulate the micromilieu of bone defects with regard to Wnt antagonists are therefore considered promising to support defect regeneration. In this study, we show the versatility of a macromer based biomaterial platform to systematically optimize covalent surface decoration with high-sulfated glycosaminoglycans (sHA3) for efficient scavenging of Wnt antagonist sclerostin. Film surfaces representing scaffold implants were cross-copolymerized from three-armed biodegradable macromers and glycidylmethacrylate and covalently decorated with various polyetheramine linkers. The impact of linker properties (size, branching) and density on sHA3 functionalization efficiency and scavenging capacities for sclerostin was tested. The copolymerized 2D system allowed for finding an optimal, cytocompatible formulation for sHA3 functionalization. On these optimized sHA3 decorated films, we showed efficient scavenging of Wnt antagonists DKK1 and sclerostin, whereas Wnt agonist Wnt3a remained in the medium of differentiating SaOS-2 and hMSC. Consequently, qualitative and quantitative analysis of hydroxyapatite staining as a measure for osteogenic differentiation revealed superior mineralization on sHA3 materials. In conclusion, we showed how our versatile material platform enables us to efficiently scavenge and inactivate Wnt antagonists from the osteogenic micromilieu. We consider this a promising approach to reduce the negative effects of Wnt antagonists in regeneration of bone defects via sHA3 decorated macromer based macroporous implants. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.