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search.filters.applied.f.access: openAccess × Author: Weingarth, Daniel × End date: 2019 × Start date: 2010 × Publisher: Cambridge : Royal Society of Chemistry ×

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Now showing 1 - 5 of 5
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    An electrochemical in situ study of freezing and thawing of ionic liquids in carbon nanopores
    (Cambridge : Royal Society of Chemistry, 2014) Weingarth, Daniel; Drumm, Robert; Foelske-Schmitz, Annette; Kotz, Rüdiger; Presser, Volker
    Room temperature ionic liquids (RTILs) are an emerging class of electrolytes enabling high cell voltages and, in return, high energy density of advanced supercapacitors. Yet, the low temperature behavior, including freezing and thawing, is little understood when ions are confined in the narrow space of nanopores. This study shows that RTILs may show a tremendously different thermal behavior when comparing bulk with nanoconfined properties as a result of the increased surface energy of carbon pore walls. In particular, a continuous increase in viscosity is accompanied by slowed-down charge-discharge kinetics as seen with in situ electrochemical characterization. Freezing reversibly collapses the energy storage ability and thawing fully restores the initial energy density of the material. For the first time, a different thermal behavior in positively and negatively polarized electrodes is demonstrated. This leads to different freezing and melting points in the two electrodes. Compared to bulk, RTILs in the confinement of electrically charged nanopores show a high affinity for supercooling; that is, the electrode may freeze during heating.
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    Carbon flow electrodes for continuous operation of capacitive deionization and capacitive mixing energy generation
    (Cambridge : Royal Society of Chemistry, 2014) Porada, S.; Weingarth, Daniel; Hamelers, H.V.M.; Bryjak, M.; Presser, Volker; Biesheuvel, P.M.
    Capacitive technologies, such as capacitive deionization and energy harvesting based on mixing energy (“capmix” and “CO2 energy”), are characterized by intermittent operation: phases of ion electrosorption from the water are followed by system regeneration. From a system application point of view, continuous operation has many advantages, to optimize performance, to simplify system operation, and ultimately to lower costs. In our study, we investigate as a step towards second generation capacitive technologies the potential of continuous operation of capacitive deionization and energy harvesting devices, enabled by carbon flow electrodes using a suspension based on conventional activated carbon powders. We show how the water residence time and mass loading of carbon in the suspension influence system performance. The efficiency and kinetics of the continuous salt removal process can be improved by optimizing device operation, without using less common or highly elaborate novel materials. We demonstrate, for the first time, continuous energy generation via capacitive mixing technology using differences in water salinity, and differences in gas phase CO2 concentration. Using a novel design of cylindrical ion exchange membranes serving as flow channels, we continuously extract energy from available concentration differences that otherwise would remain unused. These results may contribute to establishing a sustainable energy strategy when implementing energy extraction for sources such as CO2-emissions from power plants based on fossil fuels.
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    Enhanced 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, Rhett
    Supercapacitors 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.
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    Tracking the structural arrangement of ions in carbon supercapacitor nanopores using in situ small-angle X-ray scattering
    (Cambridge : Royal Society of Chemistry, 2015) Prehal, C.; Weingarth, Daniel; Perre, Emilie; Lechner, R.T.; Amenitsch, H.; Paris, O.; Presser, Volker
    The charge storage mechanism and ion arrangement inside electrically charged carbon nanopores is a very active research field with tremendous importance for advanced electrochemical technologies, such as supercapacitors or capacitive deionization. Going far beyond the state of art, we present for the first time a comprehensive study of tracking ion electrosorption in aqueous electrolytes during charging and discharging of porous carbon electrodes using in situ X-ray scattering. We provide novel and quantitative insights into the local concentration of anions and cations and demonstrate that the global number of ions within the pores does not vary during charging and discharging. In addition, we have unique access to the spatial arrangement of ions inside carbon nanopores by using a simple, yet powerful two-phase model. Applying this model to our data, we show that double-layer formation is accomplished by a unique combination of preferred counter-ion adsorption directly at the pore wall which drains ions from their local surrounding inside carbon nanopores. Effectively, this leads to a situation which globally appears as ion swapping.
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    Heat-to-current conversion of low-grade heat from a thermocapacitive cycle by supercapacitors
    (Cambridge : Royal Society of Chemistry, 2015) Härtel, Andreas; Janssen, Mathijs; Weingarth, Daniel; Presser, Volker; van Roij, Rene
    Thermal energy is abundantly available, and especially low-grade heat is often wasted in industrial processes as a by-product. Tapping into this vast energy reservoir with cost-attractive technologies may become a key element for the transition to an energy-sustainable economy and society. We propose a novel heat-to-current converter which is based on the temperature dependence of the cell voltage of charged supercapacitors. Using a commercially available supercapacitor, we observed a thermal cell-voltage rise of around 0.6 mV K-1 over a temperature window of 0 °C to 65 °C. Within our theoretical model, this can be used to operate a Stirling-like charge-voltage cycle whose efficiency is competitive to the most-efficient thermoelectric (Seebeck) engines. Our proposed heat-to-current converter is built from cheap materials, contains no moving parts, and could operate with a plethora of electrolytes which can be chosen for optimal performance at specific working temperatures. Therefore, this heat-to-current converter is interesting for small-scale, domestic, and industrial applications.