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Potential of zero total charge of platinum single crystals: a local approach to stepped surfaces vicinal to Pt(111)

Potential of zero total charge of platinum single crystals: a local approach to stepped surfaces vicinal to Pt(111)
Potential of zero total charge of platinum single crystals: a local approach to stepped surfaces vicinal to Pt(111)
The electrochemical behavior of platinum single-crystal electrodes is revisited, with special emphasis on the determination of the potential of zero charge. We show that the measure of the charge displaced during CO adsorption allows the determination of the potential of zero total charge (PZTC). The estimation of the potential of zero free charge (PZFC) is discussed, with different degrees of approximation. The application of this methodology to the study of the PZTC of platinum stepped surfaces vicinal to Pt(111) reveals a marked decrease of the PZTC due to the introduction of surface steps. This effect is interpreted as the result of the existence of markedly smaller surface potentials localized on step sites. The importance of considering local aspects of the interface is emphasized with the use of N2O reduction as a sensitive probe to the local structure of the surface. It is proposed that the different local maxima observed in the absolute value of the reduction current correspond to the local values of PZTC. It is shown that there is, in general, good agreement between the overall PZTC, obtained from the CO displacement, and that calculated from the local values inferred from the N2O reduction. Further insight is obtained with the application of the laser-induced temperature jump method. This technique is useful to calculate the potential of maximum entropy of the double-layer formation. The resulting value of this potential for Pt(111) is discussed in the light of the PZFC value obtained from different approaches. For stepped surfaces vicinal to Pt(111), two local maxima in the entropy of the double layer are observed that are close to the local PZTC values estimated from the N2O reduction. This result suggests the existence of cooperative effects in the organization of the water dipoles close to the electrode surface
1023-1935
1145-1160
Climent, V.
681168d4-6286-44c7-8681-31e3e390f95e
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Herrero, E.
463721cd-c910-407a-8c3c-85eaf6550a21
Feliu, J.
73c9bec0-7217-4730-b08c-16d03fe7a485
Climent, V.
681168d4-6286-44c7-8681-31e3e390f95e
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
Herrero, E.
463721cd-c910-407a-8c3c-85eaf6550a21
Feliu, J.
73c9bec0-7217-4730-b08c-16d03fe7a485

Climent, V., Garcia-Araez, Nuria, Herrero, E. and Feliu, J. (2006) Potential of zero total charge of platinum single crystals: a local approach to stepped surfaces vicinal to Pt(111). Russian Journal of Electrochemistry, 42 (11), 1145-1160. (doi:10.1134/S1023193506110012).

Record type: Article

Abstract

The electrochemical behavior of platinum single-crystal electrodes is revisited, with special emphasis on the determination of the potential of zero charge. We show that the measure of the charge displaced during CO adsorption allows the determination of the potential of zero total charge (PZTC). The estimation of the potential of zero free charge (PZFC) is discussed, with different degrees of approximation. The application of this methodology to the study of the PZTC of platinum stepped surfaces vicinal to Pt(111) reveals a marked decrease of the PZTC due to the introduction of surface steps. This effect is interpreted as the result of the existence of markedly smaller surface potentials localized on step sites. The importance of considering local aspects of the interface is emphasized with the use of N2O reduction as a sensitive probe to the local structure of the surface. It is proposed that the different local maxima observed in the absolute value of the reduction current correspond to the local values of PZTC. It is shown that there is, in general, good agreement between the overall PZTC, obtained from the CO displacement, and that calculated from the local values inferred from the N2O reduction. Further insight is obtained with the application of the laser-induced temperature jump method. This technique is useful to calculate the potential of maximum entropy of the double-layer formation. The resulting value of this potential for Pt(111) is discussed in the light of the PZFC value obtained from different approaches. For stepped surfaces vicinal to Pt(111), two local maxima in the entropy of the double layer are observed that are close to the local PZTC values estimated from the N2O reduction. This result suggests the existence of cooperative effects in the organization of the water dipoles close to the electrode surface

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Published date: 2006
Organisations: Electrochemistry

Identifiers

Local EPrints ID: 345810
URI: http://eprints.soton.ac.uk/id/eprint/345810
ISSN: 1023-1935
PURE UUID: 18b4ec76-5e13-4a69-aa6d-631dd730b741
ORCID for Nuria Garcia-Araez: ORCID iD orcid.org/0000-0001-9095-2379

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Date deposited: 30 Nov 2012 15:22
Last modified: 26 Nov 2019 01:36

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