Browsing by Author "Zeiger, Marco"
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- ItemCarbon onion / sulfur hybrid cathodes via inverse vulcanization for lithium sulfur batteries(Cambridge : Royal Society of Chemistry, 2017) Choudhury, Soumyadip; Srimuk, Pattarachai; Raju, Kumar; Tolosa, Aura; Fleischmann, Simon; Zeiger, Marco; Ozoemena, Kenneth I.; Borchardt, Lars; Presser, VolkerA sulfur–1,3-diisopropenylbenzene copolymer was synthesized by ring-opening radical polymerization and hybridized with carbon onions at different loading levels. The carbon onion mixing was assisted by shear in a two-roll mill to capitalize on the softened state of the copolymer. The sulfur copolymer and the hybrids were thoroughly characterized in structure and chemical composition, and finally tested by electrochemical benchmarking. An enhancement of specific capacity was observed over 140 cycles at higher content of carbon onions in the hybrid electrodes. The copolymer hybrids demonstrate a maximum initial specific capacity of 1150 mA h gsulfur−1 (850 mA h gelectrode−1) and a low decay of capacity to reach 790 mA h gsulfur−1 (585 mA h gelectrode−1) after 140 charge/discharge cycles. All carbon onion/sulfur copolymer hybrid electrodes yielded high chemical stability, stable electrochemical performance superior to conventional melt-infiltrated reference samples having similar sulfur and carbon onion content. The amount of carbon onions embedded in the sulfur copolymer has a strong influence on the specific capacity, as they effectively stabilize the sulfur copolymer and sterically hinder the recombination of sulfur species to the S8 configuration.
- ItemCarbon onion–sulfur hybrid cathodes for lithium–sulfur batteries(Cambridge : Royal Society of Chemistry, 2017) Choudhury, Soumyadip; Zeiger, Marco; Massuti-Ballester, Pau; Fleischmann, Simon; Formanek, Petr; Borchardt, Lars; Presser, VolkerIn this study, we explore carbon onions (diameter below 10 nm), for the first time, as a substrate material for lithium sulfur cathodes. We introduce several scalable synthesis routes to fabricate carbon onion–sulfur hybrids by adopting in situ and melt diffusion strategies with sulfur fractions up to 68 mass%. The conducting skeleton of agglomerated carbon onions proved to be responsible for keeping active sulfur always in close vicinity to the conducting matrix. Therefore, the hybrids are found to be efficient cathodes for Li–S batteries, yielding 97–98% Coulombic efficiency over 150 cycles with a slow fading of the specific capacity (ca. 660 mA h g−1 after 150 cycles) in long term cycle test and rate capability experiments.
- ItemElectrospinning of ultrafine metal oxide/carbon and metal carbide/carbon nanocomposite fibers(London : RSC Publishing, 2015) Atchison, Jennifer S.; Zeiger, Marco; Tolosa, Aura; Funke, Lena M.; Jäckel, Nicolas; Presser, VolkerElectrospinning has emerged as a facile technology for the synthesis of ultrafine fibers and even nanofibers of various materials. While carbon nanofibers have been extensively investigated, there have also been studies reported on metal oxide and metal carbide fibers. Yet, comparative studies, especially following the same general synthesis approach, are lacking. In our comprehensive study, we use a sol gel process by which a carrier polymer (cellulose acetate or polyvinylpyrrolidone) is mixed with titanium butoxide, zirconium(IV) acetylacetonate, or niobium n-butoxide to yield nanotextured titania/carbon, zirconia/carbon, or niobia/carbon nonwoven textiles. Carbothermal reduction between 1300 °C and 1700 °C effectively transforms the metal oxide/carbon fibers to metal carbide/carbon nanocomposite while preserving the fiber integrity. As a beneficial effect, the fiber diameter decreases compared to the as-spun state and we obtained ultrafine fibers: 294 ± 108 nm for ZrC/C, 122 ± 28 nm for TiC/C, and 65 ± 36 nm for NbC/C. The highly disordered and porous nature of the carbon matrix engulfing the metal carbide nanocrystals enables a high specific surface area of up to 450 m2 g−1 (TiC/C) after carbothermal reduction.
- ItemEmulsion soft templating of carbide-derived carbon nanospheres with controllable porosity for capacitive electrochemical energy storage(Cambridge : Royal Society of Chemistry, 2015) Oschatz, Martin; Zeiger, Marco; Jaeckel, Nicolas; Strubel, Patrick; Borchardt, Lars; Reinhold, Romy; Nickel, Winfried; Eckert, Jürgen; Presser, Volker; Kaskel, StefanA new approach to produce carbide-derived carbon nanospheres of 20-200 nm in diameter based on a novel soft-templating technique is presented. Platinum catalysis is used for the cross-linking of liquid (allylhydrido)polycarbosilane polymer chains with para-divinylbenzene within oil-in-water miniemulsions. Quantitative implementation of the pre-ceramic polymer can be achieved allowing precise control over the resulting materials. After pyrolysis and high-temperature chlorine treatment, resulting particles offer ideal spherical shape, very high specific surface area (up to 2347 m^2/g^-1), and large micro/mesopore volume (up to 1.67 cm^3/g^-1). The internal pore structure of the nanospheres is controllable by the composition of the oil phase within the miniemulsions. The materials are highly suitable for electrochemical double-layer capacitors with high specific capacitances in aqueous 1 M Na2SO4 solution (110 F/g^-1) and organic 1 M tetraethylammonium tetrafluoroborate in acetonitrile (130 F/g^-1).
- ItemEnhanced capacitance of nitrogen-doped hierarchically porous carbide-derived carbon in matched ionic liquids(Cambridge : Royal Society of Chemistry, 2015) Ewert, Julia K.; Weingarth, Daniel; Denner, Christine; Friedrich, Martin; Zeiger, Marco; Schreiber, Anna; Jäckel, Nicolas; Presser, Volker; Kempe, RhettSupercapacitors combine efficient electrical energy storage and performance stability based on fast electrosorption of electrolyte ions at charged interfaces. They are a central element of existing and emerging energy concepts. A better understanding of capacitance enhancement options is essential to exploit the full potential of supercapacitors. Here, we report a novel hierarchically structured N-doped carbon material and a significant capacitance enhancement for a specific ionic liquid. Our studies indicate that matching of the electrode material and the ionic liquid specifically leads to a constant normalized resistance of the electrode material (voltage window up to ±1 V vs. carbon) and a significant enhancement of the specific capacitance. Such effects are not seen for standard organic electrolytes, non-matched ionic liquids, or non-N-doped carbons. A higher N-doping of the electrode material improves the symmetric full cell capacitance of the match and considerably increases its long-term stability at +3 V cell voltage. This novel observance of enhanced specific capacitance for N-doped carbons with matched ionic liquid may enable a new platform for developing supercapacitors with enhanced energy storage capacity.
- 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.
- ItemGraphitization as a universal tool to tailor the potential-dependent capacitance of carbon supercapacitors(Hoboken, NJ : Wiley, 2014) Weingarth, Daniel; Zeiger, Marco; Jäckel, Nicolas; Aslan, Mesut; Feng, Guang; Presser, VolkerMost efforts to improve the energy density of supercapacitors are currently dedicated to optimized porosity or hybrid devices employing pseudocapacitive elements. Little attention has been given to the effects of the low charge carrier density of carbon on the total material capacitance. To study the effect of graphitization on the differential capacitance, carbon onion (also known as onion-like carbon) supercapacitors are chosen. The increase in density of states (DOS) related to the low density of charge carriers in carbon materials is an important effect that leads to a substantial increase in capacitance as the electrode potential is increased. Using carbon onions as a model, it is shown that this phenomenon cannot be related only to geometric aspects but must be the result of varying graphitization. This provides a new tool to significantly improve carbon supercapacitor performance, in addition to having significant consequences for the modeling community where carbons usually are approximated to be ideal metallic conductors. Data on the structure, composition, and phase content of carbon onions are presented and the correlation between electrochemical performance and electrical resistance and graphitization is shown. Highly graphitic carbons show a stronger degree of electrochemical doping, making them very attractive for enhancing the capacitance.
- ItemHigh performance stability of titania decorated carbon for desalination with capacitive deionization in oxygenated water(London : RSC Publishing, 2016) Srimuk, Pattarachai; Ries, Lucie; Zeiger, Marco; Fleischmann, Simon; Jäckel, Nicolas; Tolosa, Aura; Krüner, Benjamin; Aslan, Mesut; Presser, VolkerPerformance stability in capacitive deionization (CDI) is particularly challenging in systems with a high amount of dissolved oxygen due to rapid oxidation of the carbon anode and peroxide formation. For example, carbon electrodes show a fast performance decay, leading to just 15% of the initial performance after 50 CDI cycles in oxygenated saline solution (5 mM NaCl). We present a novel strategy to overcome this severe limitation by employing nanocarbon particles hybridized with sol–gel-derived titania. In our proof-of-concept study, we demonstrate very stable performance in low molar saline electrolyte (5 mM NaCl) with saturated oxygen for the carbon/metal oxide hybrid (90% of the initial salt adsorption capacity after 100 cycles). The electrochemical analysis using a rotating disk electrode (RDE) confirms the oxygen reduction reaction (ORR) catalytic effect of FW200/TiO2, preventing local peroxide formation by locally modifying the oxygen reduction reaction.
- ItemA high-rate aqueous symmetric pseudocapacitor based on highly graphitized onion-like carbon/ barnessite-type manganese oxide nanohybrids(Cambridge : Royal Society of Chemistry, 2015) Makgopa, Katlego; Ejikeme, Paul M.; Jafta, Charl J.; Raju, Kumar; Zeiger, Marco; Presser, Volker; Ozoemena, Kenneth I.We present a study on the pseudocapacitive properties of birnessite-type MnO2 grafted on highly graphitized onion-like carbon (OLC/MnO2). In a three-electrode setup, we evaluated two different substrates, namely a platinum disc and nickel foam. The OLC/MnO2 nanohybrid exhibited a large specific capacitance (Csp) of 295 and 323 F g−1 (at 1 A g−1) for the Pt disc and Ni foam, respectively. In addition, the Ni foam substrate exhibited much higher rate capability (power density) than the Pt disc. A symmetrical two-electrode device, fabricated with the Ni foam, showed a large Csp of 254 F g−1, a specific energy density of 5.6 W h kg−1, and a high power density of 74.8 kW kg−1. These values have been the highest for onion-based electrodes so far. The device showed excellent capacity retention when subjected to voltage-holding (floating) experiments for 50 h. In addition, the device showed a very short time constant (τ = 40 ms). This high rate handling ability of the OLC/MnO2 nanohybrid, compared to literature reports, promises new opportunities for the development of aqueous-based pseudocapacitors.
- ItemImproved Capacitive Deionization Performance of Mixed Hydrophobic / Hydrophilic Activated Carbon Electrodes(Bristol : IOP Publishing, 2016) Aslan, Mesut; Zeiger, Marco; Jäckel, Nicolas; Grobelsek, Ingrid; Weingarth, Daniel; Presser, VolkerCapacitive deionization (CDI) is a promising salt removal technology with high energy efficiency when applied to low molar concentration aqueous electrolytes. As an interfacial process, ion electrosorption during CDI operation is sensitive to the pore structure and the total pore volume of carbon electrodes limit the maximum salt adsorption capacity (SAC). Thus, activation of carbons as a widely used method to enhance the porosity of a material should also be highly attractive for improving SAC values. In our study, we use easy-to-scale and facile-to-apply CO2 activation at temperatures between 950 °C and 1020 °C to increase the porosity of commercially available activated carbon. While the pore volume and surface area can be significantly increased up to 1.51 cm3/g and 2113 m2/g, this comes at the expense of making the carbon more hydrophobic. We present a novel strategy to still capitalize the improved pore structure by admixing as received (more hydrophilic) carbon with CO2 treated (more hydrophobic) carbon for CDI electrodes without using membranes. This translates in an enhanced charge storage ability in high and low molar concentrations (1 M and 5 mM NaCl) and significantly improved CDI performance (at 5 mM NaCl). In particular, we obtain stable CDI performance at 0.86 charge efficiency with 13.1 mg/g SAC for an optimized 2:1 mixture (by mass).
- ItemIn-situ nanodiamond to carbon onion transformation in metal matrix composites(Amsterdam : Elsevier, 2018) Suarez, Sebastian; Reinert, Leander; Zeiger, Marco; Miska, Patrice; Grandthyll, Samuel; Müller, Frank; Presser, Volker; Mücklich, FrankIn the present study, nickel matrix composites reinforced with a fine distribution of nanodiamonds (6.5 vol%) as reinforcement phase are annealed in vacuum at different temperatures ranging from 750 °C to 1300 °C. This is carried out to evaluate the in-situ transformation of nanodiamonds to carbon onions within a previously densified composite. The resulting materials are thoroughly analyzed by complementary analytical methods, including Raman spectroscopy, transmission electron microscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy. The proposed in-situ transformation method presents two main benefits. On one hand, since the particle distribution of a nanodiamond-reinforced composite is significantly more homogenous than in case of the carbon onions, it is expected that the transformed particles will preserve the initial distribution features of nanodiamonds. On the other hand, the proposed process allows for the tuning of the sp3/sp2 carbon ratio by applying a single straightforward post-processing step.
- ItemInfluence of carbon substrate on the electrochemical performance of carbon/manganese oxide hybrids in aqueous and organic electrolytes(Cambridge : Royal Society of Chemistry, 2016) Zeiger, Marco; Fleischmann, Simon; Krüner, Benjamin; Tolosa, Aura; Bechtel, Stephan; Baltes, Mathias; Schreiber, Anna; Moroni, Riko; Vierrath, Severin; Thiele, Simon; Presser, VolkerManganese oxide presents very promising electrochemical properties as an electrode material in supercapacitors, but there remain important open questions to guide further development of the complex manganese oxide/carbon/electrolyte system. Our work addresses specifically the influence of carbon ordering and the difference between outer and inner porosity of carbon particles for the application in aqueous 1 M Na2SO4 and 1 M LiClO4 in acetonitrile. Birnessite-type manganese oxide was hydrothermally hybridized on two kinds of carbon onions with only outer surface area and different electrical conductivity, and conventional activated carbon with a high inner porosity. Carbon onions with a high degree of carbon ordering, high conductivity, and high outer surface area were identified as the most promising material, yielding 179 F g−1. Pore blocking in activated carbon yields unfavorable electrochemical performances. The highest specific energy of 16.4 W h kg−1 was measured for a symmetric full-cell arrangement of manganese oxide coated high temperature carbon onions in the organic electrolyte. High stability during 10 000 cycles was achieved for asymmetric full-cells, which proved as a facile way to enhance the electrochemical performance stability.
- ItemNew insights into the structure of nanoporous carbons from NMR, Raman, and pair distribution function analysis(Washington D.C. : American Chemical Society, 2015) Forse, Alexander C.; Merlet, Céline; Allan, Phoebe K.; Humphreys, Elizabeth K.; Griffin, John M.; Aslan, Mesut; Zeiger, Marco; Presser, Volker; Gogotsi, Yury; Grey, Clare P.The structural characterization of nanoporous carbons is a challenging task as they generally lack long-range order and can exhibit diverse local structures. Such characterization represents an important step toward understanding and improving the properties and functionality of porous carbons, yet few experimental techniques have been developed for this purpose. Here we demonstrate the application of nuclear magnetic resonance (NMR) spectroscopy and pair distribution function (PDF) analysis as new tools to probe the local structures of porous carbons, alongside more conventional Raman spectroscopy. Together, the PDFs and the Raman spectra allow the local chemical bonding to be probed, with the bonding becoming more ordered for carbide-derived carbons (CDCs) synthesized at higher temperatures. The ring currents induced in the NMR experiment (and thus the observed NMR chemical shifts for adsorbed species) are strongly dependent on the size of the aromatic carbon domains. We exploit this property and use computer simulations to show that the carbon domain size increases with the temperature used in the carbon synthesis. The techniques developed here are applicable to a wide range of porous carbons and offer new insights into the structures of CDCs (conventional and vacuum-annealed) and coconut shell-derived activated carbons.
- 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.
- ItemPerformance evaluation of conductive additives for activated carbon supercapacitors in organic electrolyte(Amsterdam : Elsevier, 2016) Jäckel, Nicolas; Weingarth, Daniel; Schreiber, Anna; Krüner, Benjamin; Zeiger, Marco; Tolosa Rodriguez, Aura Monserrat; Aslan, Mesut; Presser, VolkerIn this study, we investigate two different activated carbons and four conductive additive materials, all produced in industrial scale from commercial suppliers. The two activated carbons differed in porosity: one with a narrow microporous pore size distribution, the other showed a broader micro-mesoporous pore structure. Electrochemical benchmarking was done in one molar tetraethylammonium tetrafluoroborate in acetonitrile. Comprehensive structural, chemical, and electrical characterization was carried out by varied techniques. This way, we correlate the electrochemical performance with composite electrode properties, such as surface area, pore volume, electrical conductivity, and mass loading for different admixtures of conductive additives to activated carbon. The electrochemical rate handling (from 0.1 A g−1 to 10 A g−1) and long-time stability testing via voltage floating (100 h at 2.7 V cell voltage) show the influence of functional surface groups on carbon materials and the role of percolation of additive particles.
- ItemQuinone-decorated onion-like carbon/carbon fiber hybrid electrodes for high-rate supercapacitor applications(Hoboken, NJ : Wiley, 2015) Zeiger, Marco; Weingarth, Daniel; Presser, VolkerThe energy performance of carbon onions can be significantly enhanced by introducing pseudocapacitive materials, but this is commonly at the cost of power handling. In this study, a novel synergistic electrode preparation method was developed by using carbon-fiber substrates loaded with quinone-decorated carbon onions. The electrodes are free standing, binder free, extremely conductive, and the interfiber space filling overcomes the severely low apparent density commonly found for electrospun fibers. Electrochemical measurements were performed in organic and aqueous electrolytes. For both systems, a high electrochemical stability after 10 000 cycles was measured, as well as a long-term voltage floating test for the organic electrolyte. The capacitance in 1 M H2SO4 was 288 F g^−1 for the highest loading of quinones, which is similar to literature values, but with a very high power handling, showing more than 100 F g^−1 at a scan rate of 2 Vs^−1.
- ItemReview: Carbon onions for electrochemical energy storage(Cambridge : Royal Society of Chemistry, 2016) Zeiger, Marco; Jäckel, Nicolas; Mochalin, Vadym N.; Presser, VolkerCarbon onions are a relatively new member of the carbon nanomaterials family. They consist of multiple concentric fullerene-like carbon shells which are highly defective and disordered. Due to their small size of typically below 10 nm, the large external surface area, and high conductivity they are used for supercapacitor applications. As electrode materials, carbon onions provide fast charge/discharge rates resulting in high specific power but present comparatively low specific energy. They improve the performance of activated carbon electrodes as conductive additives and show suitable properties as substrates for redox-active materials. This review provides a critical discussion of the electrochemical properties of different types of carbon onions as electrode materials. It also compares the general advantages and disadvantages of different carbon onion synthesis methods. The physical and chemical properties of carbon onions, in particular nanodiamond-derived carbon onions, are described with emphasis on those parameters especially important for electrochemical energy storage systems, including the structure, conductivity, and porosity. Although the primary focus of current research is on electrode materials for supercapacitors, the use of carbon onions as conductive additives and for redox-active species is also discussed.
- ItemStructure-property relationships in mechanically stimulated Sorghum bicolor stalks(Berlin : de Gruyter, 2014) Lemloh, Marie-Louise; Pohl, Anna; Zeiger, Marco; Bauer, Petra; Weiss, Ingrid M.; Schneider, Andreas S.Mechanical properties of plants and underlying structure-property relationships are important for agricultural purposes as well as for biomimetic concepts. In this study, the effect of mechanical stimulation on morphology and bending properties of the stalk was investigated for Sorghum bicolor (Poaceae), a widely used drought-tolerant biomass grass. An experimental set-up allowing for defined growth and mechanical perturbation (flexing) during a defined growth period was designed. Mechanical properties of individual internodes of the stalk were determined by three-point bending tests. We found that the three investigated lines showed differences in their general bending strength in the non-stimulated condition. However, similar high range of bending strength values was measured for all plant lines after they underwent the mechanical stimulation procedure. The anatomy of internode cross-sections was examined to evaluate structure-property relationships. An increased thickness of the outer sclerenchymatous tissue was observed for internodes with higher bending strength values. Dried internodes fail under lower strains but showed higher bending strength. These findings show that mechanosensitivity in sorghum is dependent on genetic as well as environmental factors. The experimental system presented here offers new straight-forward possibilities for S. bicolor line selection for applications requiring mechanical strength of the stalk.
- ItemSurface structure influences contact killing of bacteria by copper(Hoboken, NJ : Wiley, 2014) Zeiger, Marco; Solioz, Marc; Edongué, Hervais; Arzt, Eduard; Schneider, Andreas S.Copper kills bacteria rapidly by a mechanism that is not yet fully resolved. The antibacterial property of copper has raised interest in its use in hospitals, in place of plastic or stainless steel. On the latter surfaces, bacteria can survive for days or even weeks. Copper surfaces could thus provide a powerful accessory measure to curb nosocomial infections. We here investigated the effect of the copper surface structure on the efficiency of contact killing of Escherichia coli, an aspect which so far has received very little attention. It was shown that electroplated copper surfaces killed bacteria more rapidly than either polished copper or native rolled copper. The release of ionic copper was also more rapid from electroplated copper compared to the other materials. Scanning electron microscopy revealed that the bacteria nudged into the grooves between the copper grains of deposited copper. The findings suggest that, in terms of contact killing, more efficient copper surfaces can be engineered.
- ItemVacuum or flowing argon: What is the best synthesis atmosphere for nanodiamond-derived carbon onions for supercapacitor electrodes?(Amsterdam : Elsevier, 2015) Zeiger, Marco; Jäckel, Nicolas; Weingarth, Daniel; Presser, VolkerWe present a comprehensive study on the influence of the synthesis atmosphere on the structure and properties of nanodiamond-derived carbon onions. Carbon onions were synthesized at 1300 and 1700 °C in high vacuum or argon flow, using rapid dynamic heating and cooling. High vacuum annealing yielded carbon onions with nearly perfect spherical shape. An increase in surface area was caused by a decrease in particle density when transitioning from sp3 to sp2 hybridization and negligible amounts of disordered carbon were produced. In contrast, carbon onions from annealing nanodiamonds in flowing argon are highly interconnected by few-layer graphene nanoribbons. The presence of the latter improves the electrical conductivity, which is reflected by an enhanced power handling ability of supercapacitor electrodes operated in an organic electrolyte (1 M tetraethylammonium tetrafluoroborate in acetonitrile). Carbon onions synthesized in argon flow at 1700 °C show a specific capacitance of 20 F/g at 20 A/g current density and 2.7 V cell voltage which is an improvement of more than 40% compared to vacuum annealing. The same effect was measured for a synthesis temperature of 1300 °C, with a 140% higher capacitance at 20 A/g for argon flow compared to vacuum annealing.