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Electrical double-layer effects on m...

Watkins, John Joseph.

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Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes./
Author:	Watkins, John Joseph.
Description:	159 p.
Notes:	Source: Dissertation Abstracts International, Volume: 66-01, Section: B, page: 0256.
Contained By:	Dissertation Abstracts International66-01B.
Subject:	Chemistry, Analytical. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3159811
ISBN:	0496932977

Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes.
Watkins, John Joseph.

Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes. - 159 p.

Source: Dissertation Abstracts International, Volume: 66-01, Section: B, page: 0256.

Thesis (Ph.D.)--The University of Utah, 2005.

This dissertation describes the investigation of the influence of the electrical double-layer on the mass- and electron-transfer rates at Pt nanometer-size electrodes. The electrical double-layer is the thin region adjacent to the metal/solution interface where a large electric field exists due to the difference of the metal and solution work functions. The thickness of the double-layer is a function of the electrolyte concentration and typically a few nanometers. Nanometer-size electrodes are used because the electrode radius determines the volume that is probed during an experiment. Hemispherical Pt electrodes were fabricated with voltammetrically measured radii approaching 1 nm. Transmission electron microscopy was used to image an electrode with a radius of 70 nm. These electrodes were further characterized by high-speed cyclic voltammetry of an adsorbed redox active monolayer to measure their electroactive areas. Voltammetric peaks corresponding to the oxidation of &sim;7,000 molecules are reported, allowing measurement of electroactive areas as small as 10 -10 cm2.

ISBN: 0496932977Subjects--Topical Terms:

586156
Chemistry, Analytical.

Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes.
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020 $a 0496932977
035 $a (UnM)AAI3159811
035 $a AAI3159811
040 $a UnM $c UnM
100 1 $a Watkins, John Joseph. $3 1904893
245 1 0 $a Electrical double-layer effects on mass transfer and electron transfer at nanometer-scale electrodes.
300 $a 159 p.
500 $a Source: Dissertation Abstracts International, Volume: 66-01, Section: B, page: 0256.
500 $a Adviser: Henry S. White.
502 $a Thesis (Ph.D.)--The University of Utah, 2005.
520 $a This dissertation describes the investigation of the influence of the electrical double-layer on the mass- and electron-transfer rates at Pt nanometer-size electrodes. The electrical double-layer is the thin region adjacent to the metal/solution interface where a large electric field exists due to the difference of the metal and solution work functions. The thickness of the double-layer is a function of the electrolyte concentration and typically a few nanometers. Nanometer-size electrodes are used because the electrode radius determines the volume that is probed during an experiment. Hemispherical Pt electrodes were fabricated with voltammetrically measured radii approaching 1 nm. Transmission electron microscopy was used to image an electrode with a radius of 70 nm. These electrodes were further characterized by high-speed cyclic voltammetry of an adsorbed redox active monolayer to measure their electroactive areas. Voltammetric peaks corresponding to the oxidation of &sim;7,000 molecules are reported, allowing measurement of electroactive areas as small as 10 -10 cm2.
520 $a Utilizing the fast mass-transfer rates inherent to nanometer-size electrodes, the heterogeneous electron-transfer rates for the oxidation of the ferrocenylmethyltrimethylammonium cation, (FcTMA+) and hexachloroiridate (III) anion (IrCl63-) were measured assuming Butler-Volmer kinetics. In the absence of supporting electrolyte, when the electrical double-layer is thickest, the electron transfer rate constant for IrCl6 3- decreased by an order of magnitude from 2.9 +/- 0.2 cm/s to 0.65 +/- 0.07 cm/s. The mass-transfer rate to nanometer-size electrodes for FcTMA+ increased while the rate for IrCl 63- decreased from the theoretical values calculated neglecting double-layer effects in the absence of supporting electrolyte. These phenomena are attributed to the influence of the electrical double layer.
520 $a The homogeneous kinetics of ion-pair formation were also studied using nanometer-size electrodes. The voltammetric position for the oxidation of the IrCl63- anion exhibits a dependence on the supporting electrolyte cation identity and concentration. The kinetics of ion-pair formation of IrCl63- with K +, Ca2+ and tetraethylammonium (TEA+) were studied at Pt disk and nanometer-size hemispherical shaped electrodes. Numerical simulations utilizing a general square-scheme mechanism for the voltammetric response suggest that the dissociation rate constant of the reactant ion pair can be determined from the voltammetric wave shape and very small electrodes.
590 $a School code: 0240.
650 4 $a Chemistry, Analytical. $3 586156
650 4 $a Chemistry, Physical. $3 560527
690 $a 0486
690 $a 0494
710 2 0 $a The University of Utah. $3 1017410
773 0 $t Dissertation Abstracts International $g 66-01B.
790 1 0 $a White, Henry S., $e advisor
790 $a 0240
791 $a Ph.D.
792 $a 2005
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3159811