Surface structural information carried by desorbing reaction products

Matsushima, Toshiyasu

doi:10.1016/j.progsurf.2007.07.001

Cited by 38 publications

(69 citation statements)

References 128 publications

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“…This can be examined only by means of the above proposed AR-REMPI-TOF method. This confirmation will make AR desorption analysis useful to separately analyze the N(a)+NO(a) → N 2 O(a) → N 2 (g) +O(a) pathway in catalyzed NO reduction [11]. The pathway will yield effective NO reduction catalysts working at low temperatures.…”

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 95%

“…• off normal on Rh(110) and Rh(100) [11]. Four-directional and inclined desorption is found on Rh(100) [30].…”

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 95%

“…CO 2 from the CO oxidation does not clear condition (2) [28,29]. Desorbing product N 2 in N 2 O(a) → N 2 (g)+O(a) on Pd(110), Rh(110) or Rh(100) fulfils all three conditions [11]. The dissociative desorption of the intermediate N 2 O(a) is the final N 2 emission process in the NO reduction on the best de-NO x metal catalysts (Pd and Rh) at lower temperatures.…”

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 97%

“…In the CO oxidation step, the product CO 2 is emitted immediately after the strong bond of Pd-O(a) in TS is broken, and the resultant spatial distribution of desorbed CO 2 is affected by the slope of the O(a) adsorption site and the symmetry around it [10]. In the N 2 desorption, the orientation of parent N 2 O molecules is preserved in the spatial distribution, i.e., desorbing N 2 is highly concentrated in an inclined way in the plane along the [001] direction, and adsorbed N 2 O is also oriented along the same direction [11]. The above structure information is mostly derived from the anisotropic spatial distribution.…”

Section: Spatial Distribution and Surface Structurementioning

confidence: 99%

“…Four-directional and inclined desorption is found on Rh(100) [30]. Adsorbed N 2 O is oriented along the [001] direction (and also the [010] direction on Rh(100) [31]) before dissociation [11]. Kokalj has predicted two adsorption forms on Pd(110) by using density functional theory with generalized gradient approximations (DFT-GGA) as shown in Fig.…”

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 99%

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An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

Matsushima

Orita

Kokalj

2013

e-J. Surf. Sci. Nanotechnol.

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In a chemical reaction, both material conversions and energy partitioning take place simultaneously. Then its mechanism must be characterized from the viewpoints on both sides. Energy partitioning in surface reactions can be examined on product desorption processes when these are repulsive. This principle is exemplified in CO(a)+O(a) → CO2(g) on Pd(110)(1×1), and its application is proposed for N2O(a) → N2(g)+O(a) on the same surface. Structural information of desorption sites and active intermediates, as well as transition states, can be delivered from desorption-and azimuth-angle dependences of physical quantities of desorbing hyper-thermal products; i.e., anisotropic distributions of their flux, and translational and internal energies.

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Section: Remarkably Anisotropic Desorptionmentioning

confidence: 95%

“…• off normal on Rh(110) and Rh(100) [11]. Four-directional and inclined desorption is found on Rh(100) [30].…”

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 95%

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 97%

Section: Spatial Distribution and Surface Structurementioning

confidence: 99%

Section: Remarkably Anisotropic Desorptionmentioning

confidence: 99%

See 3 more Smart Citations

An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

Matsushima

Orita

Kokalj

2013

e-J. Surf. Sci. Nanotechnol.

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Mechanistische Einblicke in die Bindung und Aktivierung von N₂O an Übergangsmetallzentren

Tolman

2010

Angewandte Chemie

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Da Distickstoffoxid eine bedeutende Rolle beim Ozonabbau in der Stratosphäre und als Treibhausgas spielt, besteht ein großes Interesse daran, seinen Abbau insbesondere durch Metallpromotoren zu verstehen und effizienter zu machen. Neue Erkenntnisse über die Reaktionspfade bei der N2O‐Reduktion durch Metallionen in der Gasphase sowie in heterogenen, homogenen und biologischen Katalysesystemen haben interessante Einblicke in die Struktur und Eigenschaften von Metall‐N2O‐Addukten und abgeleiteten Intermediaten gegeben. Dieses vertiefte Verständnis wird sicher zur Entwicklung von wirksameren Katalysatoren für die Verringerung der N2O‐Emissionen beitragen.

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Energy Transfer Dynamics of Formate Decomposition on Cu(110)

et al. 2017

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Energy transfer dynamics of formate (HCOO a ) decomposition on aC u(110) surface has been studied by measuring the angle-resolved intensity and translational energy distributions of CO 2 emitted from the surface in asteady-state reaction of HCOOH and O 2 .The angular distribution of CO 2 shows as harp collimation with the direction perpendicular to the surface,a srepresented by cos n q (n = 6). The mean translational energy of CO 2 is measured to be as lowas100 meV and is independent of the surface temperature (T s ). These results clearly indicate that the decomposition of formate is athermal non-equilibrium process in which al arge amount of energy released by the decomposition reaction of formate is transformed into the internal energies of CO 2 molecules.T he thermal non-equilibrium features observed in the dynamics of formate decomposition support the proposed Eley-Rideal (ER)-type mechanism for formate synthesis on copper catalysts.Energy transfer and bond rupture/formation are two important events in ac hemical reaction. [1,2] Consequently,t he reaction mechanism must be examined with both aspects in mind. Forg as-phase bimolecular reactions,e nergy transfer processes have been extensively examined by applying crossed molecular beam techniques,w here detailed dynamical parameters (such as total momentum, energy,and angular momentum, before and after the collision events) can describe the partitioning of energy into each available mode of the products. [3,4] On the other hand, characterizing the energy-transfer processes in gas-surface chemical reactions is challenging because of the large number of degrees of freedom available to the surface atoms.T oa nalyze ag assurface chemical reaction, angle-resolved (AR) analysis of the desorbed products from the surface is one of the direct methods used because it relates to the transition state (TS) structure of the reaction. [5][6][7] In this communication, we report the angle-resolved intensity and translational energy distributions of the CO 2 produced from the decomposition of formate during the steady-state reaction of HCOOH with O 2 on Cu(110).Formate (HCOO a )i sa ni mportant intermediate in the synthesis of methanol, and is formed on copper surfaces during the initial elementary CO 2 hydrogenation step, namely:C O 2 + 1/2 H 2 !HCOO a . [8][9][10] Formate synthesis is unique in terms of reaction mechanism and dynamics,a s well as its structure-insensitive kinetics.W ehave proposed an ER-type mechanism for formate synthesis,b ased on experimental kinetic analysis and theoretical calculations, [11,12] in which CO 2 directly reacts with the adsorbed hydrogen atoms (H a )o nt he copper surface without the involvement of trapping states and adsorption precursors.T his,i nt urn, implies that the formate production rate can only be enhanced by controlling the energy of the CO 2 molecules in terms of at hermal non-equilibrium character.T he dynamics of formate decomposition on copper catalysts is thus interesting as the reverse reaction of formate synthesis: HCOO a ...

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Surface structural information carried by desorbing reaction products

Cited by 38 publications

References 128 publications

An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

Mechanistische Einblicke in die Bindung und Aktivierung von N₂O an Übergangsmetallzentren

Energy Transfer Dynamics of Formate Decomposition on Cu(110)

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Surface structural information carried by desorbing reaction products

Cited by 38 publications

References 128 publications

An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

An Experimental Approach to Transition States of Surface Reactions; Energy Partitioning in Repulsive Desorption

Mechanistische Einblicke in die Bindung und Aktivierung von N2O an Übergangsmetallzentren

Energy Transfer Dynamics of Formate Decomposition on Cu(110)

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Product

Resources

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Mechanistische Einblicke in die Bindung und Aktivierung von N₂O an Übergangsmetallzentren