Ab initio study of oxygenreduction mechanism at Pt4cluster

Roudgar, Ata; Eikerling, Michael; Santen, Rutger A. van

doi:10.1039/b914570b

Cited by 53 publications

(44 citation statements)

References 42 publications

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“…Δ G pH and Δ G U are the free energy contributions due to variations in H + concentration and electrode potential, U , respectively. In this work, we consider the contributions of Δ E , Δ G pH and Δ G U to free energy and neglect the effects of other terms60. Effects of other terms will be included in a forthcoming publication.…”

Section: Methodsmentioning

confidence: 99%

Layered SiC Sheets: A Potential Catalyst for Oxygen Reduction Reaction

Zhang

Xiao

Hou

et al. 2014

Sci Rep

111

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The large-scale practical application of fuel cells cannot come true if the high-priced Pt-based electrocatalysts for oxygen reduction reaction (ORR) cannot be replaced by other efficient, low-cost, and stable electrodes. Here, based on density functional theory (DFT), we exploited the potentials of layered SiC sheets as a novel catalyst for ORR. From our DFT results, it can be predicted that layered SiC sheets exhibit excellent ORR catalytic activity without CO poisoning, while the CO poisoning is the major drawback in conventional Pt-based catalysts. Furthermore, the layered SiC sheets in alkaline media has better catalytic activity than Pt(111) surface and have potential as a metal-free catalyst for ORR in fuel cells.

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Section: Methodsmentioning

confidence: 99%

Layered SiC Sheets: A Potential Catalyst for Oxygen Reduction Reaction

Zhang

Xiao

Hou

et al. 2014

Sci Rep

111

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“…Molecular level studies have revealed that reaction steps involving formation and further reaction of chemisorbed -O and -OH on the Pt surface, including coupled electron-and proton-transfer processes, constitute the energetically most inhibited steps of the ORR mechanism. [52][53][54] The adsorption Gibbs energy of chemisorbed -O and -OH is widely considered as a yardstick in evaluating the electrocatalytic ORR activity of supported or unsupported transition metal catalysts. 55 On the one hand, chemisorbed oxygen species are intermediates of the ORR which should be formed at a high rate; on the other hand, maintaining steady high rates of ORR hinges on sufficient Pt surface sites that are free of chemisorbed oxygen species, a requirement that becomes critical if oxide species are bound too strongly.…”

Section: Discussionmentioning

confidence: 99%

Oxygen Reduction Reaction Activity and Electrochemical Stability of Thin-Film Bilayer Systems of Platinum on Niobium Oxide

et al. 2010

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Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=af7f4c9a-daa7-4ca4-bf5e-4795e8f31e04 http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=af7f4c9a-daa7-4ca4-bf5e-4795e8f31e04 Burnaby, British Columbia, V5A 1S6, Canada, and NRC Institute for Fuel Cell InnoVation, 4250 Wesbrook Mall, VancouVer, British Columbia, V6T 1W5, Canada ReceiVed: May 11, 2010; ReVised Manuscript ReceiVed: July 26, 2010 We used electrochemical testing and theoretical calculations based on density functional theory (DFT) to examine the oxygen reduction reaction (ORR) activity of platinum electrocatalyst supported on several forms of niobium oxide. Bilayer electrocatalysts were synthesized in the form of 5 nm thick Pt layers (ca. 0.01 mg/cm 2 ), deposited on 5 or 10 nm thick niobium oxide and backed by glassy carbon (GC) electrodes. The NbO and NbO 2 supports enhance the specific electrochemical activity of Pt relative to the identically synthesized baseline system of Pt on GC but have no positive effect on the mass activity. The electrochemical stability of the Pt/NbO 2 bilayer system was investigated by potential cycling with up to 2500 cyclic voltammetry (CV) cycles. After 2500 cycles, data indicates minimal electrochemical area loss. With the use of DFT calculations, we have evaluated effects of oxygen incorporation on stability, electronic structure, and electrochemical activity of Pt|Nb x O y systems. Calculations predict a transfer of electronic charge density from Nb, NbO, and NbO 2 to Pt and a reverse case for Nb 2 O 5 . However, the experimental ORR activity does not follow the trends predicted by the d-band model.

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“…25,26 The ultrasmall size of noble-metal clusters is essential for high reactivity. 27 However, NPs of 2−3 nm diameters containing 200 to 500 atoms are beyond the computational capabilities of density functional theory (DFT).…”

Section: ■ Introductionmentioning

confidence: 99%

Roles of Crystal Surface in Pt-Loaded Titania for Photocatalytic Conversion of Organic Pollutants: A First-Principle Theoretical Calculation

Chen

Wang

et al. 2015

ACS Appl. Mater. Interfaces

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Titania modified with nanosized metallic clusters is found to substantially enhance its photocatalytic capacity for renewable energy generation and environmental purification, but the underlying mechanism, especially the roles of crystal surface in noble-metal-loaded TiO2, remain unclear. In this work, such roles in the Pt-loaded anatase TiO2 for the photocatalytic conversion of nitrobenzene (NB), a model pollutant, are explored by first-principle calculations. The theoretical calculations reveal that the Pt-TiO2 complex has a higher catalytic activity toward NB conversion than pure Pt clusters, and the (001) facets of TiO2 in this complex tend to accumulate more positively charged holes and thus have a higher photocatalytic activity than the (101) facets. Furthermore, the thermodynamic and kinetic results also show that the Pt cluster loaded on the (001) surface of anatase TiO2 is favored for NB conversion in the photooxidation pathway. This work deepens our fundamental understanding on the evolution of molecule-photocatalyst interface and provides implications for designing and preparing photocatalysts.

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Ab initio study of oxygenreduction mechanism at Pt4cluster

Cited by 53 publications

References 42 publications

Layered SiC Sheets: A Potential Catalyst for Oxygen Reduction Reaction

Layered SiC Sheets: A Potential Catalyst for Oxygen Reduction Reaction

Oxygen Reduction Reaction Activity and Electrochemical Stability of Thin-Film Bilayer Systems of Platinum on Niobium Oxide

Roles of Crystal Surface in Pt-Loaded Titania for Photocatalytic Conversion of Organic Pollutants: A First-Principle Theoretical Calculation

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