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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.
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    Unraveling the Electrochemical Mechanism in Tin Oxide/MXene Nanocomposites as Highly Reversible Negative Electrodes for Lithium-Ion Batteries
    (Weinheim : Wiley-VCH, 2023) Gentile, Antonio; Arnold, Stefanie; Ferrara, Chiara; Marchionna, Stefano; Tang, Yushu; Maibach, Julia; Kübel, Christian; Presser, Volker; Ruffo, Riccardo
    Lithium-ion batteries are constantly developing as the demands for power and energy storage increase. One promising approach to designing high-performance lithium-ion batteries is using conversion/alloying materials, such as SnO2. This class of materials does, in fact, present excellent performance and ease of preparation; however, it suffers from mechanical instabilities during cycling that impair its use. One way to overcome these problems is to prepare composites with bi-dimensional materials that stabilize them. Thus, over the past 10 years, two-dimensional materials with excellent transport properties (graphene, MXenes) have been developed that can be used synergistically with conversion materials to exploit both advantages. In this work, a 50/50 (by mass) SnO2/Ti3C2Tz nanocomposite is prepared and optimized as a negative electrode for lithium-ion batteries. The nanocomposite delivers over 500 mAh g−1 for 700 cycles at 0.1 A g−1 and demonstrates excellent rate capability, with 340 mAh g−1 at 8 A g−1. These results are due to the synergistic behavior of the two components of the nanocomposite, as demonstrated by ex situ chemical, structural, and morphological analyses. This knowledge allows, for the first time, to formulate a reaction mechanism with lithium-ions that provides partial reversibility of the conversion reaction with the formation of SnO.
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    Hydrogel-Based Flexible Energy Storage Using Electrodes Based on Polypyrrole and Carbon Threads
    (Weinheim : Wiley-VCH, 2023) Ruthes, Jean G. A.; Deller, Andrei E.; Pameté, Emmanuel; Riegel‐Vidotti, Izabel C.; Presser, Volker; Vidotti, Marcio
    Developing new flexible and electroactive materials is a significant challenge to producing safe, reliable, and environmentally friendly energy storage devices. This study introduces a promising electrolyte system that fulfills these requirements. First, polypyrrole (PPy) nanotubes are electropolymerized in graphite-thread electrodes using methyl orange (MO) templates in an acidic medium. The modification increases the conductivity and does not compromise the flexibility of the electrodes. Next, flexible supercapacitors are built using hydrogel prepared from poly(vinyl alcohol) (PVA)/sodium alginate (SA) obtained by freeze–thawing and swollen with ionic solutions as an electrolyte. The material exhibits a homogenous and porous hydrogel matrix allowing a high conductivity of 3.6 mS cm−1 as-prepared while displaying great versatility, changing its electrochemical and mechanical properties depending on the swollen electrolyte. Therefore, it allows its combination with modified graphite-thread electrodes into a quasi-solid electrochemical energy storage device, achieving a specific capacitance (Cs) value of 66 F g−1 at 0.5 A g−1. Finally, the flexible device exhibits specific energy and power values of 19.9 W kg−1 and 3.0 Wh kg−1, relying on the liquid phase in the hydrogel matrix produced from biodegradable polymers. This study shows an environment friendly, flexible, and tunable quasi-solid electrolyte, depending on a simple swell experiment to shape its properties according to its application.