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    Quinone-decorated onion-like carbon/carbon fiber hybrid electrodes for high-rate supercapacitor applications
    (Hoboken, NJ : Wiley, 2015) Zeiger, Marco; Weingarth, Daniel; Presser, Volker
    The 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.
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    Reduced Faradaic Contributions and Fast Charging of Nanoporous Carbon Electrodes in a Concentrated Sodium Nitrate Aqueous Electrolyte for Supercapacitors
    (Weinheim [u.a.] : Wiley-VCH, 2019) Abbas, Qamar; Gollas, Bernhard; Presser, Volker
    The Faradaic processes related to electrochemical water reduction at the nanoporous carbon electrode under negative polarization are reduced when the concentration of aqueous sodium nitrate (NaNO3) is increased or the temperature is decreased. This effect enhances the relative contribution of ion electrosorption to the total charge storage process. Hydrogen chemisorption is reduced in aqueous 8.0 m NaNO3 due to the low degree of hydration of the Na+ cation; consequently, less free water is available for redox contributions, driving the system to exhibit electrical double-layer capacitive characteristics. Hydrogen adsorption/desorption is facilitated in 1.0 m NaNO3 due to the high molar ratio. The excess of water shifts the local pH in carbon nanopores to neutral values, giving rise to a high overpotential for dihydrogen evolution in the latter. The dilution effect on local pH shift in 1.0 m NaNO3 can be reduced by decreasing the temperature. A symmetric activated carbon cell assembled with 8.0 m NaNO3 exhibits a high capacitance and coulombic efficiency, a larger contribution of ion electrosorption to the overall charge storage process, and a stable capacitance performance at 1.6 V. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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    The Many Deaths of Supercapacitors: Degradation, Aging, and Performance Fading
    (Weinheim : Wiley-VCH, 2023) Pameté, Emmanuel; Köps, Lukas; Kreth, Fabian Alexander; Pohlmann, Sebastian; Varzi, Alberto; Brousse, Thierry; Balducci, Andrea; Presser, Volker
    High-performance electrochemical applications have expedited the research in high-power devices. As such, supercapacitors, including electrical double-layer capacitors (EDLCs) and pseudocapacitors, have gained significant attention due to their high power density, long cycle life, and fast charging capabilities. Yet, no device lasts forever. It is essential to understand the mechanisms behind performance degradation and aging so that these bottlenecks can be addressed and tailored solutions can be developed. Herein, the factors contributing to the aging and degradation of supercapacitors, including electrode materials, electrolytes, and other aspects of the system, such as pore blocking, electrode compositions, functional groups, and corrosion of current collectors are examined. The monitoring and characterizing of the performance degradation of supercapacitors, including electrochemical methods, in situ, and ex situ techniques are explored. In addition, the degradation mechanisms of different types of electrolytes and electrode materials and the effects of aging from an industrial application standpoint are analyzed. Next, how electrode degradations and electrolyte decompositions can lead to failure, and pore blocking, electrode composition, and other factors that affect the device's lifespan are examined. Finally, the future directions and challenges for reducing supercapacitors' performance degradation, including developing new materials and methods for characterizing and monitoring the devices are summarized.