Structure sensitivity of the methanation reaction: H2-induced CO dissociation on nickel surfaces

Andersson, Martin; Abild‐Pedersen, Frank; Remediakis, Ioannis N.; Bligaard, Thomas; Jones, Glenn; Engbæk, Jakob; Lytken, Ole; Horch, Sebastian; Nielsen, Linda; Sehested, Jens; Rostrup-Nielsen, J.R.; Nørskov, Jens K.; Chorkendorff, Ib

doi:10.1016/j.jcat.2007.12.016

Cited by 418 publications

(396 citation statements)

References 51 publications

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“…6 Evidence for a hydrogen-assisted pathway has been reported for Ni (Ref. 4) and Ru (Ref. 7) surfaces.…”

Section: Introductionmentioning

confidence: 90%

“…3 Theoretical and experimental works to date suggest that a hydrogen-assisted pathway should be more favorable on close-packed surfaces, whereas the carbide mechanism is preferred on stepped and corrugated surfaces. 1,[4][5][6][7][8] Theoretical studies have provided support for dissociation via H x CO intermediates on Ru(0001) (Ref. 5) and Co(0001).…”

Section: Introductionmentioning

confidence: 99%

“…Andersson et al reported dissociation at under-coordinated sites, such as steps, as being most favorable on Ni surfaces, with direct dissociation occurring under ultrahigh vacuum (UHV) conditions in the absence of hydrogen, whereas dissociation via a COH species was most favorable under methanation conditions. 4 Mitchell et al reported the formation of formyls and formaldehydes a) Author to whom correspondence should be addressed. Electronic mail: M.A.Gleeson@differ.nl.…”

Section: Introductionmentioning

confidence: 99%

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Evidence of stable high-temperature Dx-CO intermediates on the Ru(0001) surface

Ueta

Groot

Juurlink

et al. 2012

The Journal of Chemical Physics

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We demonstrate the formation of complexes involving attractive interactions between D and CO on Ru(0001) that are stable at significantly higher temperatures than have previously been reported for such intermediate species on this surface. These complexes are evident by the appearance of new desorption features upon heating of the sample. They decompose in stages as the sample temperature is increased, with the most stable component desorbing at >500 K. The D:CO ratio remaining on the surface during the final stages of desorption tends towards 1:1. The new features are populated during normally incident molecular beam dosing of D 2 on to CO pre-covered Ru(0001) surfaces (180 K) when the CO coverage exceeds 50% of the saturation value. The amount of complex formed decreases somewhat with increasing CO pre-coverage. It is almost absent in the case of dosing on to the fully saturated surface. The results are interpreted in terms of both local and long-range rearrangements of the overlayer that give rise to the observed CO coverage dependence and limit the amount of complex that can be formed.

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“…6 Evidence for a hydrogen-assisted pathway has been reported for Ni (Ref. 4) and Ru (Ref. 7) surfaces.…”

Section: Introductionmentioning

confidence: 90%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Evidence of stable high-temperature Dx-CO intermediates on the Ru(0001) surface

Ueta

Groot

Juurlink

et al. 2012

The Journal of Chemical Physics

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“…Subsequently, the structure dependence has been investigated for both the steam reforming process and the methanation reaction [10][11][12] and in both cases the structural dependence is very clear. The rate limiting step for the methanation reaction is generally believed to involve the dissociation of CO. 11,13,14 Recently, it was shown that on nickel under UHV conditions, the reaction pathway involves CO dissociation while at high pressure and in the presence of hydrogen, a COH intermediate is the precursor for dissociation. 11 The latter was deduced from measurements on catalysts combined with DFT calculations.…”

Section: Introductionmentioning

confidence: 99%

Is the methanation reaction over Ru single crystals structure dependent?

Vendelbo

Johansson

Nielsen

et al. 2011

Phys. Chem. Chem. Phys.

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The influence of monoatomic steps and defects on the methanation reaction over ruthenium has been investigated. The experiments are performed on a Ru(0 1 54) ruthenium single crystal, which contains one monoatomic step atom for each 27 terrace atoms. The methanation activity is measured at one bar of hydrogen and CO in a high pressure cell, which enables simultaneous measurements of the local reactivity of the well defined single crystal surface and the global reactivity of the entire crystal and its auxiliary support. By adding sulfur we observe that the measured activity from the well defined stepped front-side of the crystal is poisoned faster than the entire crystal containing more defects. We also observe that additional sputtering of the well-defined front-side increases the reactivity measured on the surface. Based on this, we conclude that the methanation reaction takes place on undercoordinated sites, such as steps and kinks, and that the methanation reaction is extremely structure dependent. Simulations of the flow, temperature, and product distributions in the high pressure cell are furthermore presented as supplementary information.

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“…Investigating this problem is important because, even though we know that the Hydrogen atom colliding against a metallic surface has a huge technological applications and importance for many fields of science [45][46][47] , we still do not have a deep knowledge of how this phenomenon happens. 48 This investigation is also instructive, as yet, no practical application of the newly developed formalism has been presented, although the method of exact factorization has been used to compute the time-dependence potential energy surfaces for problems that can be solved, either analytically or numerically, by alternative procedures.…”

Section: Introductionmentioning

confidence: 99%

Ab-<i>initio</i> studies of adsorbate-surface interactions

Rêgo¹

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Structure sensitivity of the methanation reaction: H2-induced CO dissociation on nickel surfaces

Cited by 418 publications

References 51 publications

Evidence of stable high-temperature Dx-CO intermediates on the Ru(0001) surface

Evidence of stable high-temperature Dx-CO intermediates on the Ru(0001) surface

Is the methanation reaction over Ru single crystals structure dependent?

Ab-<i>initio</i> studies of adsorbate-surface interactions

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