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Physical Electrochemistry Organizer: Daniel Scherson Case Western Reserve University, Cleveland, OH Organizer: Kenneth W

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Physical Electrochemistry Organizer: Daniel Scherson Case Western Reserve University, Cleveland, OH Organizer: Kenneth W Physical Electrochemistry Organizer: Daniel Scherson Case Western Reserve University, Cleveland, OH Organizer: Kenneth W. Street The NASA-Glenn Research Center, Cleveland, OH Presider: Daniel Scherson Case Western Reserve University, Cleveland, OH Session Overview: This session is devoted to all aspects of physical electrochemistry including electrocatalytic phenomena, corrosion, semiconductor electrochemistry and other topics. 1. Multiwalled Carbon Nanotube (MWCNT) as Support for PtRu Anode Catalysts of a Direct Ethanol Fuel Cell (DEFC) Susmita Singh and Jayati Datta, Department of Chemistry, Bengal Engg Sci University, Shibpur, Howrah, India DEFC is one of the most promising power sources for the near future. Since the kinetics and electro- efficiency of the process strongly depend on the noble metal formulations and their dispersion on suitable support, an intensive research is devoted to decrease the catalyst loading. This work reports an improved electro-catalytic activity for ethanol oxidation at Pt-Ru co-deposited surfaces on MWCNT support. Pt-Ru catalysts with different compositions were synthesized on pre- functionalized MWCNT by adopting sol method. The degree of surface functionalization is found to depend on the level of acid treatment. Chemical reduction of precursor salt using ethylene glycol as mild reducing agent as well as capping agent at 1400C yields catalyst particle size of few nanometers as confirmed by XRD and TEM studies. Cyclic voltammetry, polarization study and electrochemical impedance spectroscopy were employed to evaluate the electro-catalytic phenomenon over a range of H2SO4 and ethanol concentrations. A spectacular negative potential shift of more than 250 mV of the onset of ethanol oxidation was observed on the Pt-Ru catalyst in comparison to Pt alone. High mesoporous surface area of carbon nanotube can significantly increase the metal dispersion and affect particle size as well as mesoporous network of nanotubes combined with their excellent conducting properties allows a quick transport and easy accessibility of the reagent molecules to the catalytic sites enabling better performance of binary Pt-Ru system compared to Pt alone at the DEFC. 2. Thermal Energy Storage with High Energy Density and Power Density Using Macro-Encapsulated Phase Change Material Andrey Soukhojak, David Bank, Myron Maurer and Kalyan Sehanobish, The Dow Chemical Company, Midland, MI One approach to reduce CO2 emissions is to use thermal energy from renewable or waste heat sources (e.g. solar radiation, heat generated by an internal combustion engine). A major challenge for this approach is the necessity to store thermal energy for at least a few hours between 1) the times when the source’s available thermal power is high, but the need for heat is low and 2) the times when the need for thermal energy is high, but the source is not available. When electric energy is to be stored, electrochemical batteries and capacitors perform this task with high efficiency. However, the cost of electric energy storage is high due to expensive materials and the complexity of these devices. Heat (thermal energy) is a primitive form of energy, but in many applications it brings utility to the user. As with electric energy storage, the primary performance measures describing thermal energy storage (TES) are energy density and power density of the device. We report on a low-cost TES prototype that challenges the energy density and exceeds the power density of lithium ion batteries. The prototype utilizes an inorganic phase change material (PCM) in combination with metallic foil macro-encapsulation to store energy as both sensible heat and latent heat in the 20-300 °C temperature range. Working prototypes were designed which demonstrate reduction to practice for automotive and non- automotive applications. The PCM’s properties and the device architecture promise benefits in a broad range of applications, including thermal management of lithium ion batteries. 3. Theoretical Aspects of Light-Activated Microelectrodes IN Redox Electrolytes Huanfeng Zhu, Barry Miller and Daniel Scherson, Chemistry, Case Western Reserve University, Cleveland, OH Earlier studies have shown that it is possible to generate light-activated electrodes employing a focused laser impinging at normal incidence on the surface of a semiconductor electrode immersed in an electrolyte containing a redox species. Implementation of this novel concept using n-InP disk in solutions of ferrocene in well-supported acetonitrile electrolytes at high positive potentials, φbias, yielded a behavior closely resembling that of conventional metallic microelectrodes. This contribution will explore theoretically the behavior of such semiconductor-based, light-activated microelectrodes in redox electrolytes utilizing a commercial software to solve self-consistently the transport equations for solid state and solution phase species and the electrostatic potential within the semiconductor phase subject to the appropriate boundary conditions under steady state. The light- limited currents for such spatially-localized microelectrodes observed for high voltage bias, φbias, under normal irradiation and strict axisymmetric geometry were found to be proportional to the photon flux intensity. In addition, the results of these simulations afforded strong evidence that under high φbias, holes generated by the light on an n-type semiconductor escape beyond the edge of the illuminated disk, leading to a net increase in the predicted current and thus in the effective area of the light activated microelectrode. For the parameters selected for this simulation, the fraction of the total current flowing through the illuminated area of n-InP amounts to 42%. In contrast, for n-Si, an indirect band semiconductor, under the same conditions, this fraction is reduced to 27% as would be expected since the holes are generated deeper into the material. 4. Funtional Neural Stimulation: Oxygen Reduction On Supported Iridium Oxide in Neutral Media Youjiang Chen, Michelle A. Rasmussen and Daniel Scherson, Chemistry, Case Western Reserve University, Cleveland, OH Iridium oxide, IrOx, ranks among the most promising electrode materials for functional neural stimulation applications. In particular, IrOx is fully biocompatible and exhibits supercapacitive behavior, i.e. it can store reversibly large amounts of charge, which can be injected or released over very shorts period of time. Yet another attribute of this material, which has not yet been thoroughly studied, relates to its very large overpotential for dioxygen reduction. This is of special importance, as certain products of O2 reduction, e.g. superoxide and peroxide, are known to chemically attack the nerve walls impairing signal transmission. This study examines O2 reduction on IrOx supported on various substrates in phosphate buffer aqueous solutions (pH = 7). As will be shown, the potential region where IrOx exhibits pseudocapacitive properties is largely positive to the onset of O2 reduction; hence, a significant fraction of the charge stored in the film becomes available for the negative charge injection involved in neural stimulation without generation of hazardous species. 5. On the Physical Meaning of Constant Phase Element Bernard Tribollet1, Mark E. Orazem2, Isabelle Frateru3 and Vincent Vivier1, (1)Laboratoire des Interfaces et Systèmes Electrochimiques,, Université Pierre et Marie Curie, Paris cedex 05, France, (2)Department of Chemical Engineering, University of Florida, Gainesville, FL, (3)Laboratoire de Physico-Chimie des Surfaces, ENSCP, Paris, France Constant phase elements (CPE) are used extensively in electrical equivalent circuits used to analyze experimental impedance data. While CPE behavior is observed experimentally, its interpretation has been controversial for many years. However, if the CPE behavior can be considered to be evidence of frequency dispersion, its origin can be due to dispersion of the resistance, of capacitance, or both. Recent work has shown that Local Electrochemical Impedance Spectroscopy (LEIS) can be used in some cases to assess the influence of local variations on the CPE behavior seen in global measurements, and a distinction between 2D and 3D distributions could be observed. Two different formulas are proposed to relate the CPE parameters to the mean capacitance for 2D and 3D distributions. Different origins of the frequency dispersions are analyzed: geometrical effect inducing a primary current distribution, a variation of oxide layer thickness, a variation of the oxide layer resistivity according to the normal coordinate. The particular case of a CPE with an exponent of 0.5 has a particular meaning because it could be related only to a diffusion process or to a porous electrode as described by de Levie. In all cases, the high-frequency global impedance response has the appearance of a constant phase element (CPE) but can be considered to be only an apparent CPE because the CPE exponent is a function of frequency. 6. Optical Interfacial Microcalorimetry Bin Hai and Daniel Scherson, Department of Chemistry, Case Western Reserve University, Cleveland, OH A method in herein described that allows for the enthalpy of an interfacial process to be determined in situ. It is based on probe beam deflection measurements performed through the back of an optically transparent solid media which support a very thin film of a metal electrode in contact with the electrolyte solution using a laser beam propagating parallel to the interface.
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