Angle-resolved measurements of product desorption and reaction dynamics on individual sites

Matsushima, Toshiyasu

doi:10.1016/j.surfrep.2003.09.002

Cited by 87 publications

(62 citation statements)

References 183 publications

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“…11 Briefly, a reaction chamber has a mass spectrometer for measuring angle-integrated (AI) signals, low energy electron diffraction (LEED), and x-ray photoelectron spectroscopy optics. An analyzer evacuated by turbo-molecular pumps and a 25 K-cooled copper stage has another mass spectrometer for time-resolved and angleresolved (AR) measurements.…”

Section: Methodsmentioning

confidence: 99%

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Sakurai

Kondo

Nakamura

2011

The Journal of Chemical Physics

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We have investigated the effect of co-absorbed CO and reaction temperature on the angular distribution of N(2) desorption by N(2)O decomposition under the steady state of N(2)O-CO reaction on Rh(110). Spatial distributions of desorbing product N(2) emission have been measured at various surface temperatures and CO coverages. The decomposed N(2) collimates at 48°-61° off normal in the parallel plane to [001] and [110] directions, indicating that adsorbed N(2)O just before the decomposition is oriented along the [001] direction. Although the inclined and collimated N(2) desorption is always observed at any steady-state CO coverage and reaction temperature, the shape of the collimated N(2) distribution varied dependent on the co-adsorbed CO coverage. The distribution becomes sharp and shifts toward the surface normal direction with increasing CO coverage. These effects of adsorbed CO on the angular distribution of N(2) are interpreted by the collision of desorbed N(2) with co-adsorbed CO.

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Section: Methodsmentioning

confidence: 99%

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Sakurai

Kondo

Nakamura

2011

The Journal of Chemical Physics

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“…͓DOI: 10.1063/1.2918729͔ Elucidation of energy transfer dynamics and structures of transition states ͑TSs͒ is an important subject for full understanding of surface reaction. [1][2][3][4][5][6][7][8][9][10][11] Such an understanding at the atomic level is required to develop superior catalysts, electrodes, and material growth processes. Dynamics and TS structures can be studied by measurements of translational and internal ͑rotational and vibrational͒ energies of desorbing products.…”

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confidence: 99%

“…Dynamics and TS structures can be studied by measurements of translational and internal ͑rotational and vibrational͒ energies of desorbing products. 5,[12][13][14][15][16][17][18][19] Although angle-resolved ͑AR͒ measurements [5][6][7][8][9][10][11] are required to study internal energies to obtain detailed structural information, such measurements have long been lacking in thermal surface reactions because of the difficulty of experiments. In this communication, results of measurements of internal energies of AR product CO 2 in CO oxidation on Pd͑111͒ are presented.…”

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confidence: 99%

“…1,5,[11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26] Non-AR measurements of internal energies of product CO 2 have been extensively conducted by analysis of chemiluminescence from CO 2 12-17,19 and infrared ͑IR͒ absorption by CO 2 . 18 Recently, measurements of internal energies of AR CO 2 have been reported.…”

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confidence: 99%

“…T max shifts to higher values as the O 2 / CO ratio decreases because of the higher temperature required to yield vacant sites at high CO pressures. 1,5 The following AR measurements were performed for the optimum CO oxidation at T surf = 700 K and O 2 / CO=1/ 2.…”

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Mode-dependent coupling between vibration and translation of product CO2 in CO oxidation on Pd(111)

Yamanaka

2008

The Journal of Chemical Physics

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The vibrational temperatures of product CO 2 were measured in CO oxidation on Pd͑111͒ as a function of the desorption angle by means of infrared chemiluminescence. The antisymmetric vibration temperature was separately determined from the other vibrational modes from the normalized chemiluminescence intensity. The product CO 2 desorption is sharply collimated along the surface normal. The antisymmetric vibrational temperature increased from 1300 to 1600 K as the desorption angle increased from 0°to 30°, whereas the averaged vibrational temperature over bending and symmetric modes decreased from 2450 to 1530 K. From these angle dependences, an energy partitioning model in repulsive desorption is proposed. © 2008 American Institute of Physics. ͓DOI: 10.1063/1.2918729͔ Elucidation of energy transfer dynamics and structures of transition states ͑TSs͒ is an important subject for full understanding of surface reaction. [1][2][3][4][5][6][7][8][9][10][11] Such an understanding at the atomic level is required to develop superior catalysts, electrodes, and material growth processes. Dynamics and TS structures can be studied by measurements of translational and internal ͑rotational and vibrational͒ energies of desorbing products. 5,12-19Although angle-resolved ͑AR͒ measurements 5-11 are required to study internal energies to obtain detailed structural information, such measurements have long been lacking in thermal surface reactions because of the difficulty of experiments. In this communication, results of measurements of internal energies of AR product CO 2 in CO oxidation on Pd͑111͒ are presented.CO oxidation on noble metals is a prototypical surface reaction that has long attracted attention of chemists, physicists, and also mathematicians because of its practical importance and rich phenomena. 1,5,[11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26] Non-AR measurements of internal energies of product CO 2 have been extensively conducted by analysis of chemiluminescence from CO 2 [12][13][14][15][16][17]19 and infrared ͑IR͒ absorption by CO 2 .18 Recently, measurements of internal energies of AR CO 2 have been reported. 27,28 Although CO 2 has three vibrational modes ͓symmetry stretch ͑S͒, bending ͑B͒, and antisymmetric stretch ͑A͒ modes͔, in the above AR study, only rotational temperature ͑T rot ͒ and vibrational temperature ͑T vib ͒ averaged over the three modes were determined assuming T vib = T s = T b = T a ͑temperatures of S, B, and A modes͒.In this communication, mode-resolved AR measurements of vibrational energies of product CO 2 are presented. The intensity of chemiluminescence from AR product CO 2 was analyzed in comparison with that from high-temperature reference CO 2 from a newly developed molecular beam source, and the degree of excitation of A mode was separately determined from those of other vibrational modes. It was found that the excitations of A and B modes differently correlate with translational directions. In many chemical reactions, it is difficult to experimentally study the momen...

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Can NO_x reduction by CO react over carbon‐based single‐atom catalysts at low temperatures? A theoretical study

Shi

Zhang

et al. 2021

AIChE Journal

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First principles studies combined with the microkinetic analysis were performed to study the reliability and reaction mechanisms of single‐atom‐doped graphene materials in catalyzing NOx reduction with CO. By screening the 3d transition metals (Sc‐Zn) and group IV elements (Si and Ge), it was found that the Ti‐ and Co‐doped graphene sheets (TiGr and CoGr), respectively, exhibited excellent catalytic activities in the NO/NO2‐to‐N2O and the N2O‐to‐N2 processes at a relatively low temperature (450 K). Therefore, the tandem catalyst (TiGr + CoGr) can be a promising catalyst in NOx reduction with CO. It was further revealed that the combination of adsorption energy and electronegativity was a good descriptor to predict the activation energies. The obtained results provide useful information for rational design of carbon‐based single‐atom catalysts for NOx reduction by CO at low temperatures.

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Angle-resolved measurements of product desorption and reaction dynamics on individual sites

Cited by 87 publications

References 183 publications

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Mode-dependent coupling between vibration and translation of product CO2 in CO oxidation on Pd(111)

Can NO_x reduction by CO react over carbon‐based single‐atom catalysts at low temperatures? A theoretical study

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Angle-resolved measurements of product desorption and reaction dynamics on individual sites

Cited by 87 publications

References 183 publications

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Effect of co-adsorbed CO and reaction temperature on the dynamics of N2 desorption under steady-state N2O–CO reaction on Rh(110)

Mode-dependent coupling between vibration and translation of product CO2 in CO oxidation on Pd(111)

Can NOx reduction by CO react over carbon‐based single‐atom catalysts at low temperatures? A theoretical study

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Can NO_x reduction by CO react over carbon‐based single‐atom catalysts at low temperatures? A theoretical study