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Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases

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Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases. / Alves, O. B.; Hoster, H. E.; Behm, R. J.

In: Physical Chemistry Chemical Physics, Vol. 13, No. 13, 2011, p. 6010-6021.

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Alves, OB, Hoster, HE & Behm, RJ 2011, 'Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases', Physical Chemistry Chemical Physics, vol. 13, no. 13, pp. 6010-6021. https://doi.org/10.1039/c0cp01001d

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Alves, O. B. ; Hoster, H. E. ; Behm, R. J. / Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases. In: Physical Chemistry Chemical Physics. 2011 ; Vol. 13, No. 13. pp. 6010-6021.

Bibtex

@article{25e8dd6b4d1e4d2582d24313657be11a,
title = "Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases",
abstract = "We investigated the electrochemical oxidation and reduction processes on ultrahigh vacuum prepared, smooth and structurally well-characterized Ru(0001) electrodes in a CO-saturated and, for comparison, in a CO-free flowing perchloric acid electrolyte by electrochemical methods and by comparison with previous structural data. Structure and reactivity of the adsorbed layers are largely governed by a critical potential of E = 0.57 V, which determines the onset of O(ad) formation on the CO(ad) saturated surface in the positive-going scan and of O(ad) reduction in the negative-going scan. O(ad) formation proceeds via nucleation and 2D growth of high-coverage Oad islands in a surrounding CO(ad) phase, and it is connected with CO(ad) oxidation at the interface between the two phases. In the negative-going scan, mixed (CO(ad) + O(ad)) phases, most likely a (2 x 2)-(CO + 2O) and a (2 x 2)-(2CO + O), are proposed to form at E <0.57 V by reduction of the O(ad)-rich islands and CO adsorption into the resulting lower-density O(ad) structures. CO bulk oxidation rates in the potential range E > 0.57 V are low, but significantly higher than those observed during oxidation of pre-adsorbed CO in the CO-free electrolyte. We relate this to high local CO(ad) coverages due to CO adsorption in the CO-saturated electrolyte, which lowers the CO adsorption energy and thus the barrier for CO(ad) oxidation during CO bulk oxidation.",
keywords = "CARBON-MONOXIDE, ACID-SOLUTIONS, ADSORBATE INTERACTIONS, OXIDATION REACTION, ONLINE DEMS, LEED-IV, PT-RU, ELECTROOXIDATION, SURFACE, OXYGEN",
author = "Alves, {O. B.} and Hoster, {H. E.} and Behm, {R. J.}",
year = "2011",
doi = "10.1039/c0cp01001d",
language = "English",
volume = "13",
pages = "6010--6021",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Royal Society of Chemistry",
number = "13",

}

RIS

TY - JOUR

T1 - Electrochemistry at Ru(0001) in a flowing CO-saturated electrolyte-reactive and inert adlayer phases

AU - Alves, O. B.

AU - Hoster, H. E.

AU - Behm, R. J.

PY - 2011

Y1 - 2011

N2 - We investigated the electrochemical oxidation and reduction processes on ultrahigh vacuum prepared, smooth and structurally well-characterized Ru(0001) electrodes in a CO-saturated and, for comparison, in a CO-free flowing perchloric acid electrolyte by electrochemical methods and by comparison with previous structural data. Structure and reactivity of the adsorbed layers are largely governed by a critical potential of E = 0.57 V, which determines the onset of O(ad) formation on the CO(ad) saturated surface in the positive-going scan and of O(ad) reduction in the negative-going scan. O(ad) formation proceeds via nucleation and 2D growth of high-coverage Oad islands in a surrounding CO(ad) phase, and it is connected with CO(ad) oxidation at the interface between the two phases. In the negative-going scan, mixed (CO(ad) + O(ad)) phases, most likely a (2 x 2)-(CO + 2O) and a (2 x 2)-(2CO + O), are proposed to form at E <0.57 V by reduction of the O(ad)-rich islands and CO adsorption into the resulting lower-density O(ad) structures. CO bulk oxidation rates in the potential range E > 0.57 V are low, but significantly higher than those observed during oxidation of pre-adsorbed CO in the CO-free electrolyte. We relate this to high local CO(ad) coverages due to CO adsorption in the CO-saturated electrolyte, which lowers the CO adsorption energy and thus the barrier for CO(ad) oxidation during CO bulk oxidation.

AB - We investigated the electrochemical oxidation and reduction processes on ultrahigh vacuum prepared, smooth and structurally well-characterized Ru(0001) electrodes in a CO-saturated and, for comparison, in a CO-free flowing perchloric acid electrolyte by electrochemical methods and by comparison with previous structural data. Structure and reactivity of the adsorbed layers are largely governed by a critical potential of E = 0.57 V, which determines the onset of O(ad) formation on the CO(ad) saturated surface in the positive-going scan and of O(ad) reduction in the negative-going scan. O(ad) formation proceeds via nucleation and 2D growth of high-coverage Oad islands in a surrounding CO(ad) phase, and it is connected with CO(ad) oxidation at the interface between the two phases. In the negative-going scan, mixed (CO(ad) + O(ad)) phases, most likely a (2 x 2)-(CO + 2O) and a (2 x 2)-(2CO + O), are proposed to form at E <0.57 V by reduction of the O(ad)-rich islands and CO adsorption into the resulting lower-density O(ad) structures. CO bulk oxidation rates in the potential range E > 0.57 V are low, but significantly higher than those observed during oxidation of pre-adsorbed CO in the CO-free electrolyte. We relate this to high local CO(ad) coverages due to CO adsorption in the CO-saturated electrolyte, which lowers the CO adsorption energy and thus the barrier for CO(ad) oxidation during CO bulk oxidation.

KW - CARBON-MONOXIDE

KW - ACID-SOLUTIONS

KW - ADSORBATE INTERACTIONS

KW - OXIDATION REACTION

KW - ONLINE DEMS

KW - LEED-IV

KW - PT-RU

KW - ELECTROOXIDATION

KW - SURFACE

KW - OXYGEN

U2 - 10.1039/c0cp01001d

DO - 10.1039/c0cp01001d

M3 - Journal article

VL - 13

SP - 6010

EP - 6021

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 13

ER -