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- ItemMechanical Robustness of Graphene on Flexible Transparent Substrates(Washington, DC : Soc., 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.
- 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.
- ItemRecombinant perlucin derivatives influence the nucleation of calcium carbonate(London : RSC, 2016) Weber, Eva; Weiss, Ingrid M.; Cölfen, Helmut; Kellermeier, MatthiasProteins are known to play various key roles in the formation of complex inorganic solids during natural biomineralisation processes. However, in most cases our understanding of the actual underlying mechanisms is rather limited. One interesting example is perlucin, a protein involved in the formation of nacre, where it is believed to promote the crystallisation of calcium carbonate. In the present work, we have used potentiometric titration assays to systematically investigate the influence of recombinant GFP-labeled perlucin derivatives on the early stages of CaCO3 formation. Our results indicate that different parts of the protein can impact nucleation in distinct ways and act in either a retarding or promoting fashion. The most important finding is that full-length GFP-perlucin changes the nature of the initially precipitated phase and seems to favour the direct formation of crystalline polymorphs over nucleation of ACC and subsequent phase transformation, as observed in reference experiments without protein. This confirms the supposed role of perlucin in nacre biomineralisation and may rely on specific interactions between the protein and the crystal lattice of the emerging mineral phase.
- ItemAdhesion and Cellular Compatibility of Silicone-Based Skin Adhesives(Weinheim : Wiley-VCH, 2017) Fischer, Sarah C. L.; Kruttwig, Klaus; Bandmann, Vera; Hensel, René; Arzt, EduardPressure-sensitive adhesives based on silicone materials have emerging potential as adhesives in healthcare products, in particular for gentle skin adhesives. To this end, adhesion to rough skin and biocompatibility are crucial factors for a successful implementation. In this study, the mechanical, adhesive, and biological properties of the two-component poly(dimethylsiloxane) Soft Skin Adhesive MG 7-9800 (SSA, Dow Corning) have been investigated and compared to Sylgard 184. Different mixing ratios of SSA's components allow for tuning of the shear modulus, thereby modifying the adhesive properties of the polymer. To give a comprehensive insight, the authors have analyzed the interplay between pull-off stress, adhesion energy, and stretch of the adhesive films on smooth and rough surfaces. The focus is placed on the effects of substrate roughness and on low pressure oxygen plasma treatment of the adhesive films. SSA shows superior biocompatibility in in vitro cell culture experiments. High pull-off stresses in the range of 3 N cm−2 on a rough surface are achieved, promising broad application spectra for SSA-based healthcare products.
- ItemTemplated Self-Assembly of Ultrathin Gold Nanowires by Nanoimprinting for Transparent Flexible Electronics(Washington, DC : ACS Publications, 2016) Maurer, Johannes H. M.; González-García, Lola; Reiser, Beate; Kanelidis, Ioannis; Kraus, TobiasWe fabricated flexible, transparent, and conductive metal grids as transparent conductive materials (TCM) with adjustable properties by direct nanoimprinting of self-assembling colloidal metal nanowires. Ultrathin gold nanowires (diameter below 2 nm) with high mechanical flexibility were confined in a stamp and readily adapted to its features. During drying, the wires self-assembled into dense bundles that percolated throughout the stamp. The high aspect ratio and the bundling yielded continuous, hierarchical superstructures that connected the entire mesh even at low gold contents. A soft sintering step removed the ligand barriers but retained the imprinted structure. The material exhibited high conductivities (sheet resistances down to 29 Ω/sq) and transparencies that could be tuned by changing wire concentration and stamp geometry. We obtained TCMs that are suitable for applications such as touch screens. Mechanical bending tests showed a much higher bending resistance than commercial ITO: conductivity dropped by only 5.6% after 450 bending cycles at a bending radius of 5 mm.
- ItemNiobium carbide nanofibers as a versatile precursor for high power supercapacitor and high energy battery electrodes(London [u.a.] : RSC, 2016) Tolosa, Aura; Krüner, Benjamin; Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Aslan, Mesut; Grobelsek, Ingrid; Presser, VolkerThis study presents electrospun niobium carbide/carbon (NbC/C) hybrid nanofibers, with an average diameter of 69 ± 30 nm, as a facile precursor to derive either highly nanoporous niobium carbide-derived carbon (NbC–CDC) fibers for supercapacitor applications or niobium pentoxide/carbon (Nb2O5/C) hybrid fibers for battery-like energy storage. In all cases, the electrodes consist of binder-free and free-standing nanofiber mats that can be used without further conductive additives. Chlorine gas treatment conformally transforms NbC nanofiber mats into NbC–CDC fibers with a specific surface area of 1508 m2 g−1. These nanofibers show a maximum specific energy of 19.5 W h kg−1 at low power and 7.6 W h kg−1 at a high specific power of 30 kW kg−1 in an organic electrolyte. CO2 treatment transforms NbC into T-Nb2O5/C hybrid nanofiber mats that provide a maximum capacity of 156 mA h g−1. The presence of graphitic carbon in the hybrid nanofibers enabled high power handling, maintaining 50% of the initial energy storage capacity at a high rate of 10 A g−1 (64 C-rate). When benchmarked for an asymmetric full-cell, a maximum specific energy of 86 W h kg−1 was obtained. The high specific power for both systems, NbC–CDC and T-Nb2O5/C, resulted from the excellent charge propagation in the continuous nanofiber network and the high graphitization of the carbon structure.
- ItemVanadium pentoxide/carbide-derived carbon core-shell hybrid particles for high performance electrochemical energy storage(London [u.a.] : RSC, 2016) Zeiger, Marco; Ariyanto, Teguh; Krüner, Benjamin; Peter, Nicolas J.; Fleischmann, Simon; Etzold, Bastian J.M.; Presser, VolkerA novel, two step synthesis is presented combining the formation of carbide-derived carbon (CDC) and redox-active vanadium pentoxide (V2O5) in a core–shell manner using solely vanadium carbide (VC) as the precursor. In a first step, the outer part of VC particles is transformed to nanoporous CDC owing to the in situ formation of chlorine gas from NiCl2 at 700 °C. In a second step, the remaining VC core is calcined in synthetic air to obtain V2O5/CDC core–shell particles. Materials characterization by means of electron microscopy, Raman spectroscopy, and X-ray diffraction clearly demonstrates the partial transformation from VC to CDC, as well as the successive oxidation to V2O5/CDC core–shell particles. Electrochemical performance was tested in organic 1 M LiClO4 in acetonitrile using half- and asymmetric full-cell configuration. High specific capacities of 420 mA h g−1 (normalized to V2O5) and 310 mA h g−1 (normalized to V2O5/CDC) were achieved. The unique nanotextured core–shell architecture enables high power retention with ultrafast charging and discharging, achieving more than 100 mA h g−1 at 5 A g−1 (rate of 12C). Asymmetric cell design with CDC on the positive polarization side leads to a high specific energy of up to 80 W h kg−1 with a superior retention of more than 80% over 10 000 cycles and an overall energy efficiency of up to 80% at low rates.
- ItemMXene as a novel intercalation-type pseudocapacitive cathode and anode for capacitive deionization(London [u.a.] : RSC, 2016) Srimuk, Pattarachai; Kaasik, Friedrich; Krüner, Benjamin; Tolosa, Aura; Fleischmann, Simon; Jäckel, Nicolas; Tekeli, Mehmet C.; Aslan, Mesut; Suss, Matthew E.; Presser, VolkerIn this proof-of-concept study, we introduce and demonstrate MXene as a novel type of intercalation electrode for desalination via capacitive deionization (CDI). Traditional CDI cells employ nanoporous carbon electrodes with significant pore volume to achieve a large desalination capacity via ion electrosorption. By contrast, MXene stores charge by ion intercalation between the sheets of its two-dimensional nanolamellar structure. By this virtue, it behaves as an ideal pseudocapacitor, that is, showing capacitive electric response while intercalating both anions and cations. We synthesized Ti3C2-MXene by the conventional process of etching ternary titanium aluminum carbide i.e., the MAX phase (Ti3AlC2) with hydrofluoric acid. The MXene material was cast directly onto the porous separator of the CDI cell without added binder, and exhibited very stable performance over 30 CDI cycles with an average salt adsorption capacity of 13 ± 2 mg g−1.
- ItemPTFEP-Al2O3 hybrid nanowires reducing thrombosis and biofouling(Cambridge : Royal Society of Chemistry, 2019) Haidar, Ayman; Ali, Awadelkareem A.; Veziroglu, Salih; Fiutowski, Jacek; Eichler, Hermann; Müller, Isabelle; Kiefer, Karin; Faupel, Franz; Bischoff, Markus; Veith, Michael; Aktas, Oral Cenk; Abdul-Khaliq, HashimThrombosis and bacterial infection are major problems in cardiovascular implants. Here we demonstrated that a superhydrophobic surface composed of poly(bis(2,2,2-trifluoroethoxy)phosphazene) (PTFEP)-Al2O3 hybrid nanowires (NWs) is effective to reduce both platelet adhesion/activation and bacterial adherence/colonization. The proposed approach allows surface modification of cardiovascular implants which have 3D complex geometries. © 2019 The Royal Society of Chemistry.
- ItemKinetics of mRNA delivery and protein translation in dendritic cells using lipid-coated PLGA nanoparticles(London : Biomed Central, 2018) Yasar, Hanzey; Biehl, Alexander; De Rossi, Chiara; Koch, Marcus; Murgia, Xabi; Loretz, Brigitta; Lehr, Claus-MichaelBackground: Messenger RNA (mRNA) has gained remarkable attention as an alternative to DNA-based therapies in biomedical research. A variety of biodegradable nanoparticles (NPs) has been developed including lipid-based and polymer-based systems for mRNA delivery. However, both systems still lack in achieving an efficient transfection rate and a detailed understanding of the mRNA transgene expression kinetics. Therefore, quantitative analysis of the time-dependent translation behavior would provide a better understanding of mRNA's transient nature and further aid the enhancement of appropriate carriers with the perspective to generate future precision nanomedicines with quick response to treat various diseases. Results: A lipid-polymer hybrid system complexed with mRNA was evaluated regarding its efficiency to transfect dendritic cells (DCs) by simultaneous live cell video imaging of both particle uptake and reporter gene expression. We prepared and optimized NPs consisting of poly (lactid-co-glycolid) (PLGA) coated with the cationic lipid 1, 2-di-O-octadecenyl-3-trimethylammonium propane abbreviated as LPNs. An earlier developed polymer-based delivery system (chitosan-PLGA NPs) served for comparison. Both NPs types were complexed with mRNA-mCherry at various ratios. While cellular uptake and toxicity of either NPs was comparable, LPNs showed a significantly higher transfection efficiency of ~ 80% while chitosan-PLGA NPs revealed only ~ 5%. Further kinetic analysis elicited a start of protein translation after 1 h, with a maximum after 4 h and drop of transgene expression after 48 h post-transfection, in agreement with the transient nature of mRNA. Conclusions: Charge-mediated complexation of mRNA to NPs enables efficient and fast cellular delivery and subsequent protein translation. While cellular uptake of both NP types was comparable, mRNA transgene expression was superior to polymer-based NPs when delivered by lipid-polymer NPs.