Novel materials and techniques for renewable energy and biosensing applications
Item
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Title
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Novel materials and techniques for renewable energy and biosensing applications
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Identifier
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d_2009_2013:dc2cd0976a25:10451
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identifier
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10598
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Creator
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Choi, Yongki,
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Contributor
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Ramzi R. Khuri | Siu-Tung Yau
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Date
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2010
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Language
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English
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Publisher
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City University of New York.
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Subject
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Condensed matter physics | Materials science | Biophysics | Biofuel Cells | Biosensor | Renewable energy
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Abstract
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Ultrasmall (1 nm and 2.8 nm) colloidal silicon nanoparticles behave as electrocatalysts for the electrooxidation of the renewable energy sources such as ethanol, methanol and glucose. Particle-immobilized electrodes show an onset of electrocatalysis occurring at potentials between -0.4 V and 0.05 V vs. Ag/AgCl at neutral pH. Both the onset potential and the strength of electrocatalysis are dependent on particle size. Tafel measurements show that electrooxidation of the fuels is a first order reaction with the transfer of one electron. The electrocatalytic activity of the particles to the fuels undergoes at least a 50-fold increase under alkaline condition compared to under acidic condition. A significant increase in the electrocatalytic current is obtained when the electrocatalysis is performed in darkness. Prototype single-compartment and double-compartment hybrid fuel cells have been constructed and tested, using the particles as the anode electrocatalyst, in order to demonstrate the potential of the particles in fuel cell applications.;Voltage-controlled amplification of the output current of an enzymatic transistor has been demonstrated. By applying external voltage between the gating and the working electrode on which the enzyme glucose oxidase was immobilized, the biocatalytic output current was increased significantly, allowing the detection limit of glucose to be lowered from the milli-molar to the zepto-molar level. The current amplification was reversibly controlled by the applied voltage. Applying this technique to the ethanol-alcohol dehydrogenase system showed similar results. The enzyme's bio-specificity was preserved in the presence of the field. The detector, with its output current controlled by the voltage applied at a third electrode, behaves as a field-effect transistor, whose current-generating mechanism is the conversion of analytes to products using an enzyme as catalyst. In addition, voltage-controlled reaction kinetics of biological catalysis is achieved using the microperoxidase-11 and hydrogen peroxide system. The interfacial electron transfer of the system was manipulated by applying the voltage to the electrode. The manipulated electron transfer causes kinetic parameters of the catalysis to acquire nonlinear dependences on the voltage. The nonlinearity indicates the feasibility of effectively controlling the efficiency of a bio-catalytic reaction or a conversion process using the voltage.
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Type
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dissertation
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Source
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2009_2013.csv
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degree
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Ph.D.
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Program
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Physics
