Steady-state oxidation of carbon monoxide over supported noble metals with particular reference to platinum

Cant, Noel W.; Hicks, P.C.; Lennon, B. S.

doi:10.1016/0021-9517(78)90085-4

Cited by 231 publications

(106 citation statements)

References 19 publications

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“…The partial pressures and temperatures leading to this high activity state of the RuO 2 (110) surface in the calculations, and even the absolute TOF values under these conditions, agree extremely well with detailed experimental studies measuring the steady-state activity in the temperature range from 300-600 K and both at highpressures and in UHV 56,57,58 . This statement comprises already the emerging consensus that this Ru oxide also forms at the surface of Ru model catalysts in highpressure environments 52,53 , i.e.…”

Section: E Surface Oxidation and Sabatier Principlesupporting

confidence: 81%

“…the high activity that was originally ascribed to the Ru substrate was in fact due to RuO 2 56,57 . With this understanding a puzzle is finally resolved that had bothered surface scientists for quite a while: For a long time the high CO oxidation reactivity of supported Ru catalysts 56 , as well as of Ru(0001) single crystals 57 at high-pressures stood in sharp contrast to exceedingly low turnover rates observed under UHV conditions 59 , thus representing a nice example of a socalled "pressure gap" system 60 .…”

Section: E Surface Oxidation and Sabatier Principlementioning

confidence: 99%

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Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

Reuter

2007

Nanocatalysis

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If metal surfaces are exposed to sufficiently oxygen-rich environments, oxides start to form. Important steps in this process are the dissociative adsorption of oxygen at the surface, the incorporation of O atoms into the surface, the formation of a thin oxidic overlayer and the growth of the once formed oxide film. For the oxidation process of late transition metals (TM), recent experimental and theoretical studies provided a quite intriguing atomic-scale insight: The formed initial oxidic overlayers are not merely few atomic-layer thin versions of the known bulk oxides, but can exhibit structural and electronic properties that are quite distinct to the surfaces of both the corresponding bulk metals and bulk oxides. If such nanometer or even sub-nanometer surface oxide films are stabilized in applications, new functionalities not scalable from the known bulk materials could correspondingly arise. This can be particularly important for oxidation catalysis, where technologically relevant gas phase conditions are typically quite oxygen-rich. In such environments surface oxides may even form naturally in the induction period, and actuate then the reactive steady-state behavior that has traditionally been ascribed to the metal substrates. Corresponding aspects are reviewed by focusing on recent progress in the modeling and understanding of the oxidation behavior of late TMs, using particularly the late 4d series from Ru to Ag to discuss trends.

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Section: E Surface Oxidation and Sabatier Principlesupporting

confidence: 81%

Section: E Surface Oxidation and Sabatier Principlementioning

confidence: 99%

Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

Reuter

2007

Nanocatalysis

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“…Ar). CO conversion was determined from online mass spectrometric (MS, Omnistar, Pfeiffer) data obtained by following m/z signals corresponding to CO (28), O 2 (32), Ar (40) and CO 2 (44).…”

Section: Methodsmentioning

confidence: 99%

“…220 °C in the present case) and a high activity regime (above ca. 220 °C) [28,29]. The low activity regime was characterized by CO conversion increasing exponentially up to ca.…”

Section: Evaluation Of the Spectroscopy Cellmentioning

confidence: 99%

High energy X-ray diffraction and IR spectroscopy of Pt/Al2O3 during CO oxidation in a novel catalytic reactor cell

Marchionni

Kambolis

Nachtegaal

et al. 2017

Catalysis, Structure & Reactivity

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c École polytechnique fédérale de lausanne (ePFl), institute for Chemical science and engineering, lausanne, switzerland ABSTRACTThe operando methodology dictates not only that catalysts are analysed during reaction while activity and selectivity are monitored by analytical methods, but also that the cell in which the measurement is carried out performs as a catalytic reactor. A cell (Chiarello et al., Rev. Sci. Inst. 85 (2014) 074102) used to conduct spectroscopy and diffraction measurements under operando conditions was tested for CO oxidation on a 2 wt% Pt/Al 2 O 3 catalyst and compared with measurements in a conventional quartz catalytic reactor to demonstrate its suitability to derive kinetic data. High energy X-ray diffraction data were collected during alternate CO and O 2 pulses under differential conditions to demonstrate the extent of loss of order of the Pt particles upon exposure to the O 2 pulse. The presence of a surface oxide species places the catalyst in a higher activity regime compared to the fully reduced one.

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“…Particular interest in the CO oxidation over Ru was originally triggered by work on supported catalysts by Cant et al [3]. Under UHV conditions their "ruthenium" catalyst exhibited by far the lowest activity among the studied late transition metals, while under reactant pressures of the order of atmospheres the situation was reversed, and a superior activity compared with Pt, Rh or Pd was measured.…”

Section: Oxide Formation In the Reactive Environmentmentioning

confidence: 99%

Insight into a Pressure and Materials Gap: CO Oxidation at "Ruthenium" Catalysts

Reuter¹

2006

Oil & Gas Science and Technology - Rev. IFP

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Résumé -Impact de la pression et de l'état du matériau sur la réactivité : oxydation de CO avec des catalyseurs de « ruthénium » -Des travaux expérimentaux et théoriques récents sur l'oxydation du CO avec des catalyseurs au ruthenium offrent un apercu fascinant sur les origines microscopiques des « gouffres » des pressions et des matériaux, sujet souvent controversé entres les études réalisées dans des conditions réalistes de pression et celles réalisées sous ultravide (UHV). En se concentrant sur le catalyseur modèle Ru(0001), le système considéré présente en fait deux composants importants relatifs à ce sujet. En premier lieu, un environnement riche en oxygène transforme le matériau Ru en RuO 2 . Ainsi, des études antérieures sur la pression ambiante portant sur les catalyseurs au « ruthénium » se concentraient en fait sur un film d'oxyde formé à la surface. En second lieu, même après que le RuO 2 se soit formé, la composition de surface varie fortement selon la pression ; il faut également noter que sur le RuO 2 (110) formé, il y a une phase de surface de basse pression qui est couramment étudiée sous UHV, mais qui présente peu d'éléments en commun avec la situation où le catalyseur est actif. (0001) Abstract -Insight into a Pressure and Materials Gap: CO Oxidation at "Ruthenium" CatalystsRecent experimental and theoretical work on the CO oxidation reaction at "ruthenium" catalysts provides intriguing insight into the microscopic origins behind the frequently discussed pressure and materials gap between studies performed in ultra-high vacuum (UHV) and under realistic pressure conditions. Focusing on the Ru

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Steady-state oxidation of carbon monoxide over supported noble metals with particular reference to platinum

Cited by 231 publications

References 19 publications

Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

High energy X-ray diffraction and IR spectroscopy of Pt/Al2O3 during CO oxidation in a novel catalytic reactor cell

Insight into a Pressure and Materials Gap: CO Oxidation at "Ruthenium" Catalysts

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