128 research outputs found
Influence of Structure and Surface Chemistry of Porous Carbon Electrodes on Supercapacitor Performance
Electrochemical double layer capacitors, which rely on electrosorption of ions in nanostructured carbon electrodes, can supplement or even replace traditional batteries in energy harvesting and storage applications. While supercapacitors offer > 10 kW/kg power densities, their ~5 Wh/kg energy densities are insufficient for many automotive and grid storage applications. Most prior efforts have focused on novel high-performing ionic liquid electrolytes and porous carbons with tunable pore diameters and high specific surface areas. However, existing research lacks fundamental understanding of the influence of surface heterogeneity and disorder, such as graphitic defects and functional groups, on key electrosorption properties at electrode-electrolyte interfaces. These interactions significantly impact charge accumulation densities, ion transport mechanisms, and electrolyte breakdown processes. Subsequently, they must be investigated to optimize ion screening, charge mobilities, and operating voltage windows of the devices. The research in this dissertation examined the influence of surface functional groups and structural ordering on capacitance, electrosorption dynamics, and electrochemical stability of external and internal surface of carbon electrodes. High-temperature vacuum annealing, air oxidation, hydrogenation, and amination were used to tune pore surface compositions and decouple key structural and chemical properties of carbide-derived carbons. The approach combined materials characterization by a variety of techniques, neutron scattering studies of ion dynamics, electrochemical testing, and MD simulations to investigate the fundamental intermolecular interactions and dynamics of ions electrosorption in different pore architectures and on planar graphene surfaces. Contrary to expected results and existing theories, defect removal via defunctionalization and graphitization decreased capacitance. Hydrogenated surfaces benefitted electrosorption, while oxygen-containing groups, which increased the wettability and ionophilicity of electrodes, positively impacted capacitance by decreasing ion densities in confined pores and improving electrolyte diffusion. The influence of surface defects strongly depended on ion properties, carbon particle size and internal-to-external surface ratio, porosity, and ion confinement. These fundamental concepts were applied to several energy storage systems, including high-performance coarse-grained and core-shell carbide derived carbon electrodes, a novel in situ spectroelectrochemical analysis method, and design of an environmentally benign "green" supercapacitor.Ph.D., Materials Science and Engineering -- Drexel University, 201
Highlights from Faraday Discussion 172: Carbon in electrochemistry, Sheffield, UK, July 2014.
Traditionally, Faraday Discussions have been very true to their name, focussing genuinely on healthy, in-depth, and fruitful discussions rather than just serving as a platform for one to one researcher interaction and collaboration. So the first experience of a Faraday Discussion is always an eye-opener about how lively conference discussions can become. The format follows that presenters submit full papers a few months in advance which are lightly reviewed before all the papers are circulated to each of the registered participants. All participants arrive at the conference prepared with their queries and arguments after having read the circulated manuscripts. At the conference the authors present their work for five minutes each followed by extensive discussion of 20–25 minutes, which is practically a "live peer-review". This experience of a discussion-cum-peer review with participants ranging for PhD students to experts in the relevant field is both a daunting and a very enriching experience at the same time. This has been the trend since the first Faraday Discussions held in London in 1907 in London which debated "osmotic pressure", and this format clearly sets it apart from any other conference to date. All discussions form part of the peer review process and are sequentially recorded and published with the accepted manuscripts
Reaction of perfluoro carbanions with mercury trifluoroacetate and trifluoromethylmercury trifluoroacetate
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