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- ItemTime‐Dependent Cation Selectivity of Titanium Carbide MXene in Aqueous Solution(Weinheim : Wiley-VCH, 2022) Wang, Lei; Torkamanzadeh, Mohammad; Majed, Ahmad; Zhang, Yuan; Wang, Qingsong; Breitung, Ben; Feng, Guang; Naguib, Michael; Presser, VolkerElectrochemical ion separation is a promising technology to recover valuable ionic species from water. Pseudocapacitive materials, especially 2D materials, are up-and-coming electrodes for electrochemical ion separation. For implementation, it is essential to understand the interplay of the intrinsic preference of a specific ion (by charge/size), kinetic ion preference (by mobility), and crystal structure changes. Ti3C2Tz MXene is chosen here to investigate its selective behavior toward alkali and alkaline earth cations. Utilizing an online inductively coupled plasma system, it is found that Ti3C2Tz shows a time-dependent selectivity feature. In the early stage of charging (up to about 50 min), K+ is preferred, while ultimately Ca2+ and Mg2+ uptake dominate; this unique phenomenon is related to dehydration energy barriers and the ion exchange effect between divalent and monovalent cations. Given the wide variety of MXenes, this work opens the door to a new avenue where selective ion-separation with MXene can be further engineered and optimized.
- ItemLight-Regulated Angiogenesis via a Phototriggerable VEGF Peptidomimetic(Weinheim : Wiley-VCH, 2021) Nair, Roshna V.; Farrukh, Aleeza; del Campo, AránzazuThe application of growth factor based therapies in regenerative medicine is limited by the high cost, fast degradation kinetics, and the multiple functions of these molecules in the cell, which requires regulated delivery to minimize side effects. Here a photoactivatable peptidomimetic of the vascular endothelial growth factor (VEGF) that allows the light-controlled presentation of angiogenic signals to endothelial cells embedded in hydrogel matrices is presented. A photoresponsive analog of the 15-mer peptidomimetic Ac-KLTWQELYQLKYKGI-NH2 (abbreviated PQK) is prepared by introducing a 3-(4,5-dimethoxy-2-nitrophenyl)-2-butyl (DMNPB) photoremovable protecting group at the Trp4 residue. This modification inhibits the angiogenic potential of the peptide temporally. Light exposure of PQK modified hydrogels provide instructive cues to embedded endothelial cells and promote angiogenesis at the illuminated sites of the 3D culture, with the possibility of spatial control. PQK modified photoresponsive biomaterials offer an attractive approach for the dosed delivery and spatial control of pro-angiogenic factors to support regulated vascular growth by just using light as an external trigger.
- ItemWhen Ultimate Adhesive Mechanism Meets Ultimate Anti‐Fouling Surfaces - Polydopamine Versus SLIPS: Which One Prevails?(Weinheim : Wiley-VCH, 2020) Prieto-López, Lizbeth Ofelia; Herbeck-Engel, Petra; Yang, Li; Wu, Qian; Li, Juntang; Cui, JiaxiWhat happens when the extremely adhesive and versatile chemistry of polydopamine (PDA) is in contact with the extremely slippery surfaces known as slippery liquid‐infused porous substrates (SLIPS)? Inspired by the pitcher plant, SLIPS possess excellent repellence against a variety of complex liquids and have been proposed as promising antifouling surfaces because of their successful performance even in marine environments. In the counterpart, inspired by the adhesive proteins enabling the strong adhesion of mussels to multiple substrates, PDA has been extensively studied for its ability to adhere on nearly every type of substrate. The interaction between various SLIPS systems and the highly fouling medium from the oxidative polymerization of dopamine is explored here. A PDA coating is observed on all the SLIPS evaluated, modifying their hydrophobicity in most cases. In‐depth study of silicone‐based SLIPS shows that hydrophobicity of PDA coated SLIPS partially recovers with time due to percolation of the lubricant through the coating. “Strongly” bound PDA species are attributed to the formation of dopamine‐polydimethylsiloxane species on the crosslinked matrix, rendering a coating that withstands repeated washing steps in various solvents including water, hexane, and toluene. The results not only satisfy scientific curiosity but also imply a strategy to modify/bond SLIPS.
- ItemEnhancing the Stabilization Potential of Lyophilization for Extracellular Vesicles(Weinheim : Wiley-VCH, 2021) Trenkenschuh, Eduard; Richter, Maximilian; Heinrich, Eilien; Koch, Marcus; Fuhrmann, Gregor; Friess, WolfgangExtracellular vesicles (EV) are an emerging technology as immune therapeutics and drug delivery vehicles. However, EVs are usually stored at −80 °C which limits potential clinical applicability. Freeze-drying of EVs striving for long-term stable formulations is therefore studied. The most appropriate formulation parameters are identified in freeze-thawing studies with two different EV types. After a freeze-drying feasibility study, four lyophilized EV formulations are tested for storage stability for up to 6 months. Freeze-thawing studies revealed improved colloidal EV stability in presence of sucrose or potassium phosphate buffer instead of sodium phosphate buffer or phosphate-buffered saline. Less aggregation and/or vesicle fusion occurred at neutral pH compared to slightly acidic or alkaline pH. EVs colloidal stability can be most effectively preserved by addition of low amounts of poloxamer 188. Polyvinyl pyrrolidone failed to preserve EVs upon freeze-drying. Particle size and concentration of EVs are retained over 6 months at 40 °C in lyophilizates containing 10 mm K- or Na-phosphate buffer, 0.02% poloxamer 188, and 5% sucrose. The biological activity of associated beta-glucuronidase is maintained for 1 month, but decreased after 6 months. Here optimized parameters for lyophilization of EVs that contribute to generate long-term stable EV formulations are presented. © 2021 The Authors. Advanced Healthcare Materials published by Wiley-VCH GmbH
- ItemBending as Key Mechanism in the Tactile Perception of Fibrillar Surfaces(Weinheim : Wiley-VCH, 2021) Gedsun, Angelika; Sahli, Riad; Meng, Xing; Hensel, René; Bennewitz, RolandThe 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.
- ItemIncreasing Antibacterial Efficiency of Cu Surfaces by targeted Surface Functionalization via Ultrashort Pulsed Direct Laser Interference Patterning(Weinheim : Wiley-VCH, 2020) Müller, Daniel W.; Lößlein, Sarah; Terriac, Emmanuel; Brix, Kristina; Siems, Katharina; Moeller, Ralf; Kautenburger, Ralf; Mücklich, FrankCopper (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
- ItemHybrid Dielectric Films of Inkjet-Printable Core-Shell Nanoparticles(Weinheim : Wiley-VCH, 2021) Buchheit, Roman; Kuttich, Björn; González-García, Lola; Kraus, TobiasA new type of hybrid core-shell nanoparticle dielectric that is suitable for inkjet printing is introduced. Gold cores (dcore ≈ 4.5 nm diameter) are covalently grafted with thiol-terminated polystyrene (Mn = 11000 Da and Mn = 5000 Da) and used as inks to spin-coat and inkjet-print dielectric films. The dielectric layers have metal volume fractions of 5 to 21 vol% with either random or face-centered-cubic structures depending on the polymer length and grafting density. Films with 21 vol% metal have dielectric constants of 50@1 Hz. Structural and electrical characterization using transmission electron microscopy, small-angle X-ray scattering, and impedance spectroscopy indicates that classical random capacitor-resistor network models partially describe this hybrid material but fail at high metal fractions, where the covalently attached shell prevents percolation and ensures high dielectric constants without the risk of dielectric breakdown. A comparison of disordered to ordered films indicates that the network structure affects dielectric properties less than the metal content. The applicability of the new dielectric material is demonstrated by formulating inkjet inks and printing devices. An inkjet-printed capacitor with an area of 0.79 mm2 and a 17 nm thick dielectric had a capacitance of 2.2±0.1 nF@1 kHz .
- ItemEngineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications(Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, EduardReversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
- ItemHigh‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries(Weinheim : Wiley-VCH, 2022) Lin, Ling; Wang, Kai; Sarkar, Abhishek; Njel, Christian; Karkera, Guruprakash; Wang, Qingsong; Azmi, Raheleh; Fichtner, Maximilian; Hahn, Horst; Schweidler, Simon; Breitung, BenHigh-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.
- ItemYields and Immunomodulatory Effects of Pneumococcal Membrane Vesicles Differ with the Bacterial Growth Phase(Weinheim : Wiley-VCH, 2021) Mehanny, Mina; Kroniger, Tobias; Koch, Marcus; Hoppstädter, Jessica; Becher, Dörte; Kiemer, Alexandra K.; Lehr, Claus-Michael; Fuhrmann, GregorStreptococcus pneumoniae infections are a leading cause of death worldwide. Bacterial membrane vesicles (MVs) are promising vaccine candidates because of the antigenic components of their parent microorganisms. Pneumococcal MVs exhibit low toxicity towards several cell lines, but their clinical translation requires a high yield and strong immunogenic effects without compromising immune cell viability. MVs are isolated during either the stationary phase (24 h) or death phase (48 h), and their yields, immunogenicity and cytotoxicity in human primary macrophages and dendritic cells have been investigated. Death-phase vesicles showed higher yields than stationary-phase vesicles. Both vesicle types displayed acceptable compatibility with primary immune cells and several cell lines. Both vesicle types showed comparable uptake and enhanced release of the inflammatory cytokines, tumor necrosis factor and interleukin-6, from human primary immune cells. Proteomic analysis revealed similarities in vesicular immunogenic proteins such as pneumolysin, pneumococcal surface protein A, and IgA1 protease in both vesicle types, but stationary-phase MVs showed significantly lower autolysin levels than death-phase MVs. Although death-phase vesicles produced higher yields, they lacked superiority to stationary-phase vesicles as vaccine candidates owing to their similar antigenic protein cargo and comparable uptake into primary human immune cells.