In this work, the oxygen reduction reaction (ORR) on tellurium-modified Pt(111) surfaces has been studied. Adsorption of Te adatoms on Pt(111) progressively shifts toward less positive values of both the ORR reaction onset and the half-wave potential in 0.1M HClO4 for 0 < θTe < 0.25. However, at θTe > 0.25, the ORR activity increases relative to the one at θTe < 0.25, but remains lower than that on clean Pt(111). Results were analyzed in light of simulations of kinetic currents as a function of θTe, calculated by employing a simple mean field model including both site blocking and electronic effects. Inside this framework, experimental data are best explained by considering that oxygenated Te species inhibit the ORR by either negatively modifying adsorption energies of reaction intermediates or combined site-blocking and electronic effects. A redox ORR catalysis due to redox properties of Te adatoms is discarded. Contrarily, in 0.05M H2SO4, a positive catalytic effect has been found, interpreted in terms of a competitive adsorption–desorption mechanism involving the replacement of adsorbed sulfate by Te adatoms. On the other hand, despite the strong site-blocking effect on Hads and OHads adsorption by Te adatoms, it appears that the reduced Te–Pt(111) adlayer does not inhibit the reaction, suggesting different active sites for Hads and OHads adsorption and for the rate-determining step of the ORR mechanism.
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7 April 2020
Research Article|
April 03 2020
Structure effects on electrocatalysts. Oxygen reduction on Te-modified Pt(111) surfaces: Site-blocking vs electronic effects
Special Collection:
Interfacial Structure and Dynamics for Electrochemical Energy Storage
Ana María Gómez-Marín
;
Ana María Gómez-Marín
a)
1
Department of Chemistry, Division of Fundamental Sciences (IEF), Technological Institute of Aeronautics (ITA)
, São José dos Campos CEP: 12228-900, SP, Brazil
a)Authors to whom correspondence should be addressed: agomezma@ita.br. Tel.: +55 12 3947 6852 and juan.feliu@ua.es. Tel.: +34 965 909 301. Fax: +34 965 903 537
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Valentín Briega-Martos
;
Valentín Briega-Martos
2
Instituto de Electroquímica, Universidad de Alicante
, Apt 99, E-03080 Alicante, Spain
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Juan M. Feliu
Juan M. Feliu
a)
2
Instituto de Electroquímica, Universidad de Alicante
, Apt 99, E-03080 Alicante, Spain
a)Authors to whom correspondence should be addressed: agomezma@ita.br. Tel.: +55 12 3947 6852 and juan.feliu@ua.es. Tel.: +34 965 909 301. Fax: +34 965 903 537
Search for other works by this author on:
a)Authors to whom correspondence should be addressed: agomezma@ita.br. Tel.: +55 12 3947 6852 and juan.feliu@ua.es. Tel.: +34 965 909 301. Fax: +34 965 903 537
Note: This paper is part of the JCP Special Topic on Interfacial Structure and Dynamics for Electrochemical Energy Storage.
J. Chem. Phys. 152, 134702 (2020)
Article history
Received:
February 04 2020
Accepted:
March 10 2020
Citation
Ana María Gómez-Marín, Valentín Briega-Martos, Juan M. Feliu; Structure effects on electrocatalysts. Oxygen reduction on Te-modified Pt(111) surfaces: Site-blocking vs electronic effects. J. Chem. Phys. 7 April 2020; 152 (13): 134702. https://doi.org/10.1063/5.0003125
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