A Molecular Beam Study of the Kinetics of the Catalytic Reduction of NO by CO on Rh(111) Single-Crystal Surfaces

Gopinath, Chinnakonda S.; Zaera, Francisco

doi:10.1006/jcat.1999.2561

Cited by 61 publications

(83 citation statements)

References 43 publications

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“…To probe the oxygen transition states in CO oxidation, isotope labeling was used [17]. Figure 6 shows schematically how these ideas have been used to find the answer to the question of low-temperature carbon dioxide production using MB techniques [9,10,12,37]. the apparent activation energy of these reactions are quite different (figure 7(c)).…”

Section: Molecular Beam Studies: Model Titrations and Steady-state mentioning

confidence: 99%

“…Isothermal, non-linear dynamic processes with H 2 +O 2 , CO+O 2 , NO+H 2 mixtures have been studied on Pd, Rh, Ir and Pt tips in the 10 )7 to 10 )3 torr total pressure regime [3,4], and with molecular beams using single crystals [5][6][7][8][9][10][11][12]. When considering CO oxidation reactions, it is worth noticing that oxygen adsorbs only molecularly at low temperatures (O 2ads , T~100 K), and dissociates above 170 K. Moreover, heating O 2 -dosed surfaces above 170 K results in the desorption of some of the O 2ads molecules.…”

Section: Introductionmentioning

confidence: 99%

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Study of the low-temperature reaction between CO and O2 over Pd and Pt surfaces

et al. 2005

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Field electron microscopy (FEM), high-resolution electron energy loss spectroscopy (HREELS), molecular beams (MB) and temperature-programmed reaction (TPR) have been applied to the study of the kinetics of CO oxidation at low temperature, and to determine the roles of subsurface atomic oxygen (O sub ) and surface reconstruction in self-oscillatory phenomena, on Pd(111), Pd(110) and Pt(100) single crystals and on Pd and Pt tip surfaces. It was found that high local concentrations of adsorbed CO during the transition from a Pt(100)-hex reconstructed surface to the unreconstructed 1·1 phase apparently prevents oxygen atoms from occupying hollow sites on the surface, and leads to the appearance of a weakly bound active adsorbed atomic oxygen (O ads ) state in an on-top or bridge position. It was also inferred that subsurface oxygen O sub on the Pd(110) surface may play an important role in the formation of new active sites for the weakly bound O ads atoms. Experiments with 18 O isotope labeling clearly show that the weakly bound atomic oxygen is the active form of oxygen that reacts with CO to form CO 2 at T~140-160 K. Sharp tips of Pd and Pt, several hundreds angstroms in diameter, were used to perform in situ investigations of dynamic surface processes. The principal conclusion from those studies was that non-linear reaction kinetics is not restricted to macroscopic planes since: (i) planes as small as~200 Å in diameter show the same non-linear kinetics as larger flat surfaces; (ii) regular waves appear under conditions leading to reaction rate oscillations; (iii) the propagation of reaction-diffusion waves involves the participation of different crystal nanoplanes via an effective coupling between adjacent planes.

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Section: Molecular Beam Studies: Model Titrations and Steady-state mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Study of the low-temperature reaction between CO and O2 over Pd and Pt surfaces

et al. 2005

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“…Studies of NO-CO reaction have been carried out on Pt(1 0 0) [30][31][32][33][34][35][36][37], Pt(1 1 1) [38], Pt(1 1 2) [39], Pd(1 0 0) [40], Pd(1 1 0) [41][42][43][44], Pd(1 1 1) [42,43,45,[46][47][48][49][50][51][52][53], Rh(1 0 0) [54], Rh(1 1 0) [54], Rh(1 1 1) [54][55][56][57][58][59][60][61][62][63][64][65], Ir(1 1 1) [66], Ir(2 1 1) [67], Cu(0 0 1) [68], Ag(1 1 1) [69], Pd/Cu(1 1 1) [48], Fe/Rh(1 0 0) [55], Rh/CeO x (1 1 1) [70], Pd/MgO(1 0 0) [71,72], Pt-Rh/TiO 2 (1 1 0) [73]...…”

Section: No-co Reactionmentioning

confidence: 99%

Surface science studies of selective catalytic reduction of NO: Progress in the last ten years

Griffiths

Norton

2009

Surface Science

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“…1,2 The catalytic reduction of NO to N 2 on rhodium has been heavily investigated both experimentally [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] and theoretically [22][23][24][25][26][27][28][29][30][31][32][33][34][35] for many years. The key steps of this reaction have long been thought to be the breaking of the N-O bond in NO upon chemisorption on the metal and the subsequent recombination of surface nitrogen atoms to form N 2 .…”

Section: Introductionmentioning

confidence: 99%

“…23 A reaction window appears for the square lattice only when N atoms are allowed to diffuse on the surface 24 or when the NO and CO adsorbed species are allowed to desorb. 25 Recent experimental kinetic measurements on the reduction of NO on Rh͑111͒ performed by using a molecular beam method [17][18][19][20][21] have cast some doubts on the validity of the traditionally accepted mechanism described above. Specifically, it was found that when a 14 N-covered Rh͑111͒ surface is exposed to 15 NOϩCO beams, the molecular nitrogen produced always contains at least one 15 N atom.…”

Section: Introductionmentioning

confidence: 99%

Lattice-gas study of the kinetics of catalytic conversion of NO–CO mixtures on rhodium surfaces

Bustos

Gopinath

Uñac

et al. 2001

The Journal of Chemical Physics

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Lattice-gas study of the kinetics of the catalytic NO-CO reaction on rhodium surfaces. II. The effect of nitrogen surface islands A fast x-ray photoelectron spectroscopy study of the NO-H 2 reaction over Rh(533): Identifying surface speciesThe kinetics of the catalytic reduction of NO by CO on Rh͑111͒ was simulated by using a lattice-gas model and a Monte Carlo algorithm. These simulations were designed to incorporate some new experimental results, which reveal that the formation of a N-NO intermediate is necessary for molecular nitrogen production. The steady-state phase diagram for the overall NO reduction reaction was studied in terms of several parameters representing different reaction schemes. It was found that, under the assumptions made in the model, an Eley-Rideal mechanism which includes a NO͑gas͒ϩN͑ads͒→N 2 ͑gas͒ϩO͑ads͒ step is absolutely necessary to be able to sustain a steady-state catalytic regime.

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A Molecular Beam Study of the Kinetics of the Catalytic Reduction of NO by CO on Rh(111) Single-Crystal Surfaces

Cited by 61 publications

References 43 publications

Study of the low-temperature reaction between CO and O2 over Pd and Pt surfaces

Study of the low-temperature reaction between CO and O2 over Pd and Pt surfaces

Surface science studies of selective catalytic reduction of NO: Progress in the last ten years

Lattice-gas study of the kinetics of catalytic conversion of NO–CO mixtures on rhodium surfaces

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