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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.
- ItemEnhanced electrochemical energy storage by nanoscopic decoration of endohedral and exohedral carbon with vanadium oxide via atomic layer deposition(Washington D.C. : American Chemical Society, 2016) Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Krüner, Benjamin; Grobelsek, Ingrid; Formanek, Petr; Choudhury, Soumyadip; Weingarth, Daniel; Presser, VolkerAtomic layer deposition (ALD) is a facile process to decorate carbon surfaces with redox-active nanolayers. This is a particularly attractive route to obtain hybrid electrode materials for high performance electrochemical energy storage applications. Using activated carbon and carbon onions as representatives of substrate materials with large internal or external surface area, respectively, we have studied the enhanced energy storage capacity of vanadium oxide coatings. While the internal porosity of activated carbon readily becomes blocked by obstructing nanopores, carbon onions enable the continued deposition of vanadia within their large interparticle voids. Electrochemical benchmarking in lithium perchlorate in acetonitrile (1 M LiClO4) showed a maximum capacity of 122 mAh/g when using vanadia coated activated carbon and 129 mAh/g for vanadia coated carbon onions. There is an optimum amount of vanadia between 50 and 65 wt % for both substrates that results in an ideal balance between redox-activity and electrical conductivity of the hybrid electrode. Assembling asymmetric (charge balanced) full-cells, a maximum specific energy of 38 Wh/kg and 29 Wh/kg was found for carbon onions and activated carbon, respectively. The stability of both systems is promising, with a capacity retention of ∼85–91% after 7000 cycles for full-cell measurements.
- 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.
- ItemGold nanorods with conjugated polymer ligands: sintering-free conductive inks for printed electronics(Cambridge : Royal Society of Chemistry, 2016) Reiser, B.; González-García, L.; Kanelidis, I.; Maurer, J.H.M.; Kraus, T.Metal-based nanoparticle inks for printed electronics usually require sintering to improve the poor electron transport at particle-particle interfaces. The ligands required for colloidal stability act as insulating barriers and must be removed in a post-deposition sintering step. This complicates the fabrication process and makes it incompatible with many flexible substrates. Here, we bind a conjugated, electrically conductive polymer on gold nanorods (AuNRs) as a ligand. The polymer, poly[2-(3-thienyl)-ethyloxy-4-butylsulfonate] (PTEBS), provides colloidal stability and good electron transport properties to stable, sintering-free inks. We confirm that the polymer binds strongly through a multidentate binding motif and provides superior colloidal stability in polar solvents over months by IR and Raman spectrometry and zeta potential measurements. We demonstrate that the developed ligand exchange protocol is directly applicable to other polythiophenes such as poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS). Films of AuNRs coated with above polymers reached conductivities directly after deposition comparable to conventional metal inks after ligand removal and retained their conductivity for at least one year when stored under ambient conditions.
- 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.
- ItemVanadia–titania multilayer nanodecoration of carbon onions via atomic layer deposition for high performance electrochemical energy storage(Cambridge : Royal Society of Chemistry, 2016) Fleischamann, Simon; Tolosa, Aura; Zieger, Marco; Krüner, Benjamin; Peter, Nicolas J.; Grobelsek, Ingrid; Quade, Antje; Kruth, Angela; Presser, VolkerAtomic layer deposition has proven to be a particularly attractive approach for ecorating mesoporous carbon substrates with redox active metal oxides for lectrochemical energy storage. This study, for the first time, capitalizes on the cyclic character of atomic layer deposition to obtain highly conformal and atomically controlled decoration of carbon onions with alternating stacks of vanadia and titania. The addition of 25 mass% TiO2 leads to expansion of the VO2 unit cell, thus greatly enhancing lithium intercalation capacity and kinetics. Electrochemical characterization revealed an ultrahigh discharge capacity of up to 382 mA h g^-1 of the composite electrode (554 mA h g^-1 per metal oxide) with an impressive capacity retention of 82 mA h g^-1 (120 mA h g^-1 per metal oxide) at a high discharge rate of 20 A g^-1 or 52C. Stability benchmarking showed stability over 3000 cycles when discharging to a reduced potential of ^-1.8 V vs. carbon. These capacity values are among the highest reported for any metal oxide system, while in addition, upercapacitor-like power performance and longevity are achieved. At a device level, high specific energy and power of up to 110 W h kg^-1 and 6 kW kg^-1, respectively, were achieved when employing the hybrid material as anode versus activated carbon cathode.
- 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.
- ItemFabrication of silicon nanowire arrays by near-field laser ablation and metal-assisted chemical etching(Bristol : IOP Publishing, 2016) Brodoceanu, Daniel; Alhmoud, Hashim Z.; Elnathan, Roey; Delalat, Bahman; Voelcker, Nicolas H.; Kraus, TobiasWe present an elegant route for the fabrication of ordered arrays of vertically-aligned silicon nanowires with tunable geometry at controlled locations on a silicon wafer. A monolayer of transparent microspheres convectively assembled onto a gold-coated silicon wafer acts as a microlens array. Irradiation with a single nanosecond laser pulse removes the gold beneath each focusing microsphere, leaving behind a hexagonal pattern of holes in the gold layer. Owing to the near-field effects, the diameter of the holes can be at least five times smaller than the laser wavelength. The patterned gold layer is used as catalyst in a metal-assisted chemical etching to produce an array of vertically-aligned silicon nanowires. This approach combines the advantages of direct laser writing with the benefits of parallel laser processing, yielding nanowire arrays with controlled geometry at predefined locations on the silicon surface. The fabricated VA-SiNW arrays can effectively transfect human cells with a plasmid encoding for green fluorescent protein.