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Mechanical Robustness of Graphene on Flexible Transparent Substrates
2016, Kang, Moon H., Prieto López, Lizbeth O., Chen, Bingan, Teo, Ken, Williams, John A., Milne, William I., Cole, Matthew T.
This study reports on a facile and widely applicable method of transferring chemical vapor deposited (CVD) graphene uniformly onto optically transparent and mechanically flexible substrates using commercially available, low-cost ultraviolet adhesive (UVA) and hot-press lamination (HPL). We report on the adhesion potential between the graphene and the substrate, and we compare these findings with those of the more commonly used cast polymer handler transfer processes. Graphene transferred with the two proposed methods showed lower surface energy and displayed a higher degree of adhesion (UVA: 4.40 ± 1.09 N/m, HPL: 0.60 ± 0.26 N/m) compared to equivalent CVD-graphene transferred using conventional poly(methyl methacrylate) (PMMA: 0.44 ± 0.06 N/m). The mechanical robustness of the transferred graphene was investigated by measuring the differential resistance as a function of bend angle and repeated bend–relax cycles across a range of bend radii. At a bend angle of 100° and a 2.5 mm bend radius, for both transfer techniques, the normalized resistance of graphene transferred on polyethylene terephthalate (PET) was around 80 times less than that of indium–tin oxide on PET. After 104 bend cycles, the resistance of the transferred graphene on PET using UVA and HPL was found to be, on average, around 25.5 and 8.1% higher than that of PMMA-transferred graphene, indicating that UVA- and HPL-transferred graphene are more strongly adhered compared to PMMA-transferred graphene. The robustness, in terms of maintained electrical performance upon mechanical fatigue, of the transferred graphene was around 60 times improved over ITO/PET upon many thousands of repeated bending stress cycles. On the basis of present production methods, the development of the next-generation of highly conformal, diverse form factor electronics, exploiting the emerging family of two-dimensional materials, necessitates the development of simple, low-cost, and mechanically robust transfer processes; the developed UVA and HPL approaches show significant potential and allow for large-area-compatible, near-room temperature transfer of graphene onto a diverse range of polymeric supports.
Increasing Antibacterial Efficiency of Cu Surfaces by targeted Surface Functionalization via Ultrashort Pulsed Direct Laser Interference Patterning
2020, Müller, Daniel W., Lößlein, Sarah, Terriac, Emmanuel, Brix, Kristina, Siems, Katharina, Moeller, Ralf, Kautenburger, Ralf, Mücklich, Frank
Copper (Cu) exhibits great potential for application in the design of antimicrobial contact surfaces aiming to reduce pathogenic contamination in public areas as well as clinically critical environments. However, current application perspectives rely purely on the toxic effect of emitted Cu ions, without considering influences on the interaction of pathogenic microorganisms with the surface to enhance antimicrobial efficiency. In this study, it is investigated on how antibacterial properties of Cu surfaces against Escherichia coli can be increased by tailored functionalization of the substrate surface by means of ultrashort pulsed direct laser interference patterning (USP-DLIP). Surface patterns in the scale range of single bacteria cells are fabricated to purposefully increase bacteria/surface contact area, while parallel modification of the surface chemistry allows to involve the aspect of surface wettability into bacterial attachment and the resulting antibacterial effectivity. The results exhibit a delicate interplay between bacterial adhesion and the expression of antibacterial properties, where a reduction of bacterial cell viability of up to 15-fold can be achieved for E. coli on USP-DLIP surfaces in comparison to smooth Cu surfaces. Thereby, it can be shown how the antimicrobial properties of copper surfaces can be additionally enhanced by targeted surface functionalization. © 2020 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
Development of bioactive catechol functionalized nanoparticles applicable for 3D bioprinting
2021, Puertas-Bartolomé, María, Włodarczyk-Biegun, Małgorzata K., del Campo, Aránzazu, Vázquez-Lasa, Blanca, San Román, Julio
Efficient wound treatments to target specific events in the healing process of chronic wounds constitute a significant aim in regenerative medicine. In this sense, nanomedicine can offer new opportunities to improve the effectiveness of existing wound therapies. The aim of this study was to develop catechol bearing polymeric nanoparticles (NPs) and to evaluate their potential in the field of wound healing. Thus, NPs wound healing promoting activities, potential for drug encapsulation and controlled release, and further incorporation in a hydrogel bioink formulation to fabricate cell-laden 3D scaffolds are studied. NPs with 2 and 29 M % catechol contents (named NP2 and NP29) were obtained by nanoprecipitation and presented hydrodynamic diameters of 100 and 75 nm respectively. These nanocarriers encapsulated the hydrophobic compound coumarin-6 with 70% encapsulation efficiency values. In cell culture studies, the NPs had a protective effect in RAW 264.7 macrophages against oxidative stress damage induced by radical oxygen species (ROS). They also presented a regulatory effect on the inflammatory response of stimulated macrophages and promoted upregulation of the vascular endothelial growth factor (VEGF) in fibroblasts and endothelial cells. In particular, NP29 were used in a hydrogel bioink formulation using carboxymethyl chitosan and hyaluronic acid as polymeric matrices. Using a reactive mixing bioprinting approach, NP-loaded hydrogel scaffolds with good structural integrity, shape fidelity and homogeneous NPs dispersion, were obtained. The in vitro catechol NPs release profile of the printed scaffolds revealed a sustained delivery. The bioprinted scaffolds supported viability and proliferation of encapsulated L929 fibroblasts over 14 days. We envision that the catechol functionalized NPs and resulting bioactive bioink presented in this work offer promising advantages for wound healing applications, as they: 1) support controlled release of bioactive catechol NPs to the wound site; 2) can incorporate additional therapeutic functions by co-encapsulating drugs; 3) can be printed into 3D scaffolds with tailored geometries based on patient requirements.
Molecular stiffness cues of an interpenetrating network hydrogel for cell adhesion
2022, Li, Bin, Çolak, Arzu, Blass, Johanna, Han, Mitchell, Zhang, Jingnan, Zheng, Yijun, Jiang, Qiyang, Bennewitz, Roland, del Campo, Aránzazu
Understanding cells' response to the macroscopic and nanoscale properties of biomaterials requires studies in model systems with the possibility to tailor their mechanical properties and different length scales. Here, we describe an interpenetrating network (IPN) design based on a stiff PEGDA host network interlaced within a soft 4-arm PEG-Maleimide/thiol (guest) network. We quantify the nano- and bulk mechanical behavior of the IPN and the single network hydrogels by single-molecule force spectroscopy and rheological measurements. The IPN presents different mechanical cues at the molecular scale, depending on which network is linked to the probe, but the same mechanical properties at the macroscopic length scale as the individual host network. Cells attached to the interpenetrating (guest) network of the IPN or to the single network (SN) PEGDA hydrogel modified with RGD adhesive ligands showed comparable attachment and spreading areas, but cells attached to the guest network of the IPN, with lower molecular stiffness, showed a larger number and size of focal adhesion complexes and a higher concentration of the Hippo pathway effector Yes-associated protein (YAP) than cells linked to the PEGDA single network. The observations indicate that cell adhesion to the IPN hydrogel through the network with lower molecular stiffness proceeds effectively as if a higher ligand density is offered. We claim that IPNs can be used to decipher how changes in ECM design and connectivity at the local scale affect the fate of cells cultured on biomaterials.
Elastomeric Optical Waveguides by Extrusion Printing
2022, Feng, Jun, Zheng, Yijun, Jiang, Qiyang, Włodarczyk‐Biegun, Małgorzata K., Pearson, Samuel, del Campo, Aránzazu
Advances in optogenetics and the increasing use of implantable devices for therapies and health monitoring are driving demand for compliant, biocompatible optical waveguides and scalable methods for their manufacture. Molding, thermal drawing, and dip-coating are the most prevalent approaches in recent literature. Here the authors demonstrate that extrusion printing at room temperature can be used for continuous fabrication of compliant optical waveguides with polydimethylsiloxane (PDMS) core and crosslinked Pluronic F127-diacrylate (Pluronic-DA) cladding. The optical fibers are printed from fluid precursor inks and stabilized by physical interactions and photoinitiated crosslinking in the Pluronic-DA. The printed fibers show optical loss values of 0.13–0.34 dB cm–1 in air and tissue within the wavelength range of 405–520 nm. The fibers have a Young's Modulus (Pluronic cladding) of 150 kPa and can be stretched to more than 5 times their length. The optical loss of the fibers shows little variation with extension. This work demonstrates how printing can simplify the fabrication of compliant and stretchable devices from materials approved for clinical use. These can be of interest for optogenetic or photopharmacology applications in extensible tissues, like muscles or heart.
High‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries
2022, Lin, Ling, Wang, Kai, Sarkar, Abhishek, Njel, Christian, Karkera, Guruprakash, Wang, Qingsong, Azmi, Raheleh, Fichtner, Maximilian, Hahn, Horst, Schweidler, Simon, Breitung, Ben
High-entropy sulfides (HESs) containing 5 equiatomic transition metals (M), with different M:S ratios, are prepared by a facile one-step mechanochemical approach. Two new types of single-phase HESs with pyrite (Pa-3) and orthorhombic (Pnma) structures are obtained and demonstrate a homogeneously mixed solid solution. The straightforward synthesis method can easily tune the desired metal to sulfur ratio for HESs with different stoichiometries, by utilizing the respective metal sulfides, even pure metals, and sulfur as precursor chemicals. The structural details and solid solution nature of HESs are studied by X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, electron energy loss spectroscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectroscopy, and Mössbauer spectroscopy. Since transition metal sulfides are a very versatile material class, here the application of HESs is presented as electrode materials for reversible electrochemical energy storage, in which the HESs show high specific capacities and excellent rate capabilities in secondary Li-ion batteries.
Nanotopography mediated osteogenic differentiation of human dental pulp derived stem cells
2017, Bachhuka, Akash, Delalat, Bahman, Ghaemi, Soraya Rasi, Gronthos, Stan, Voelcker, Nicolas H., Vasilev, Krasimir
Advanced medical devices, treatments and therapies demand an understanding of the role of interfacial properties on the cellular response. This is particularly important in the emerging fields of cell therapies and tissue regeneration. In this study, we evaluate the role of surface nanotopography on the fate of human dental pulp derived stem cells (hDPSC). These stem cells have attracted interest because of their capacity to differentiate to a range of useful lineages but are relatively easy to isolate. We generated and utilized density gradients of gold nanoparticles which allowed us to examine, on a single substrate, the influence of nanofeature density and size on stem cell behavior. We found that hDPSC adhered in greater numbers and proliferated faster on the sections of the gradients with higher density of nanotopography features. Furthermore, greater surface nanotopography density directed the differentiation of hDPSC to osteogenic lineages. This study demonstrates that carefully tuned surface nanotopography can be used to manipulate and guide the proliferation and differentiation of these cells. The outcomes of this study can be important in the rational design of culture substrates and vehicles for cell therapies, tissue engineering constructs and the next generation of biomedical devices where control over the growth of different tissues is required.
Bending as Key Mechanism in the Tactile Perception of Fibrillar Surfaces
2021, Gedsun, Angelika, Sahli, Riad, Meng, Xing, Hensel, René, Bennewitz, Roland
The touching of fibrillar surfaces elicits a broad range of affective reactions, which range from the adverse stinginess of a stiff bristle brush to the pleasant feel of velvet. To study the tactile perception of model fibrillar surfaces, a unique set of samples carrying dense, regular arrays of cylindrical microfibrils with high aspect ratio made from different elastomer materials have been created. Fibril length and material compliance are varied independently such that their respective influence on tactile perception can be elucidated. This work finds that the tactile perception of similarity between samples is dominated by bending of the fibrils under sliding touch. The results demonstrate that variations of material stiffness and of surface structure are not necessarily perceived independently by touch. In the case of fibrillar elastomer surfaces, it is rather the ratio of fibril length and storage modulus which determines fibril bending and becomes the dominant tactile dimension. Visual access to the sample during tactile exploration improves the tactile perception of fibril bendability. Experiments with colored samples show a distraction by color in participants’ decisions regarding tactile similarity only for yellow samples of outstanding brightness.
Regulating Bacterial Behavior within Hydrogels of Tunable Viscoelasticity
2022, Bhusari, Shardul, Sankaran, Shrikrishnan, del Campo, Aránzazu
Engineered living materials (ELMs) are a new class of materials in which living organism incorporated into diffusive matrices uptake a fundamental role in material's composition and function. Understanding how the spatial confinement in 3D can regulate the behavior of the embedded cells is crucial to design and predict ELM's function, minimize their environmental impact and facilitate their translation into applied materials. This study investigates the growth and metabolic activity of bacteria within an associative hydrogel network (Pluronic-based) with mechanical properties that can be tuned by introducing a variable degree of acrylate crosslinks. Individual bacteria distributed in the hydrogel matrix at low density form functional colonies whose size is controlled by the extent of permanent crosslinks. With increasing stiffness and elastic response to deformation of the matrix, a decrease in colony volumes and an increase in their sphericity are observed. Protein production follows a different pattern with higher production yields occurring in networks with intermediate permanent crosslinking degrees. These results demonstrate that matrix design can be used to control and regulate the composition and function of ELMs containing microorganisms. Interestingly, design parameters for matrices to regulate bacteria behavior show similarities to those elucidated for 3D culture of mammalian cells.
Precipitate number density determination in microalloyed steels by complementary atom probe tomography and matrix dissolution
2022, Weber, Louis, Webel, Johannes, Mücklich, Frank, Kraus, Tobias
Particle number densities are a crucial parameter in the microstructure engineering of microalloyed steels. We introduce a new method to determine nanoscale precipitate number densities of macroscopic samples that is based on the matrix dissolution technique (MDT) and combine it with atom probe tomography (APT). APT counts precipitates in microscopic samples of niobium and niobium-titanium microalloyed steels. The new method uses MDT combined with analytical ultracentrifugation (AUC) of extracted precipitates, inductively coupled plasma–optical emission spectrometry, and APT. We compare the precipitate number density ranges from APT of 137.81 to 193.56 × 1021 m−3 for the niobium steel and 104.90 to 129.62 × 1021 m−3 for the niobium-titanium steel to the values from MDT of 2.08 × 1021 m−3 and 2.48 × 1021 m−3. We find that systematic errors due to undesired particle loss during extraction and statistical uncertainties due to the small APT volumes explain the differences. The size ranges of precipitates that can be detected via APT and AUC are investigated by comparison of the obtained precipitate size distributions with transmission electron microscopy analyses of carbon extraction replicas. The methods provide overlapping resulting ranges. MDT probes very large numbers of small particles but is limited by errors due to particle etching, while APT can detect particles with diameters below 10 nm but is limited by small-number statistics. The combination of APT and MDT provides comprehensive data which allows for an improved understanding of the interrelation between thermo-mechanical controlled processing parameters, precipitate number densities, and resulting mechanical-technological material properties. Graphical abstract: [Figure not available: see fulltext.]
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