The interaction of NO with stepped Rh surfaces

Janssen, N.M.H.; Cholach, A. R.; Ikai, Masamichi; Tanaka, Kenichi; Nieuwenhuys, B.E.

doi:10.1016/s0039-6028(97)00141-6

Cited by 28 publications

(10 citation statements)

References 63 publications

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“…When comparing the reactivity of the (111) step with the (100) step, two things will play a role, first of all, the activity and, second, the rate of deactivation (poisoning) during the reaction. Experimental and computational studies of the dissociation of the NO molecule on stepped rhodium and ruthenium surfaces indicate that both the (111) and the (100) steps are well able to dissociate NO. − Because NO and nitrogen are similar diatomic molecules with a strong internal bond, one would also expect nitrogen to dissociate (or recombine) well on both types of steps. A principle feature of (100) steps is that they bind adsorbates more strongly than (111) steps.…”

Section: Model and Methodsmentioning

confidence: 99%

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

et al. 2005

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Lateral adsorbate-adsorbate interactions result in variation of the desorption rate constants with coverage. This effect can be studied in great detail from the shape of a multi-isotherm. To produce the multi-isotherm, the temperature is increased in a (semi)stepwise fashion to some temperature, followed by maintaining this temperature for a prolonged time. Then, the temperature is stepped to a higher value and held constant at this new temperature. This cycle is continued until all of the adsorbates have desorbed. Using a detailed kinetic Monte Carlo model and an optimization algorithm based on Evolutionary Strategy, we are able to reproduce the shape of the experimentally measured multi-isotherm of nitrogen on Rh(111) and obtain the lateral interactions between the nitrogen atoms.

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Section: Model and Methodsmentioning

confidence: 99%

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

et al. 2005

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“…Among the noble metals of TWCs, Rh plays a dominant role in NO reduction because of its high catalytic reactivity toward NO decomposition. Intensive experimental and theoretical studies on NO adsorption and dissociation have been carried out on low-index Rh single-crystal surfaces [Rh(100), Rh(110), Rh(111)] − and stepped surfaces [Rh(211), Rh(221), Rh(311), Rh(321), Rh(410), Rh(511), Rh(533)], ,− with and without H 2 . The results showed that the surface activity of Rh is dependent on different surface structures.…”

Section: Introductionmentioning

confidence: 99%

NO Reduction by H₂ on the Rh(111) and Rh(221) Surfaces: A Mechanistic and Kinetic Study

Huai

Wen

et al. 2016

J. Phys. Chem. C

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Periodic density functional theory (DFT) was used to investigate the selective catalytic reduction of NO by H 2 (H 2 SCR) on Rh(111) and stepped Rh(221) surfaces. The stepped Rh(221) surface exhibits a higher reactivity for NO reduction than the Rh(111) surface. NO dissociation on the Rh(221) surface exhibits almost no effect in the presence of H 2 , whereas predosed H atoms slightly inhibit NO dissociation on Rh(111). Microkinetic calculations further predicted the product selectivity for H 2 SCR at different temperatures and pressures. It was found that, under ultrahigh-vacuum (UHV) conditions, NH 3 is the only Ncontaining product on Rh(111), consistent with the experimental observations, whereas on the Rh(221) surface, N 2 O formation is predominant at low temperatures, and N 2 becomes main product above 480 K. Under near-atmospheric-pressure conditions, the product selectivity on the Rh(111) surface exhibits almost no change, whereas N 2 O is the dominant product on Rh(221) throughout the whole temperature range. The present study indicates that the NO dissociation activity and product selectivity are strongly dependent on both the Rh surface structure and the experimental conditions.

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“…Because of its ability to convert NO to N 2 with high selectivity, rhodium has become an integral part of automotive catalytic converters. − To gain a better understanding of the mechanism behind this conversion, numerous surface science studies have been carried out using techniques such as low-energy electron diffraction (LEED), temperature programmed desorption (TPD), X-ray photoelectron spectroscopy (XPS), and high-resolution electron energy loss spectroscopy (HREELS). These studies have generally focused on the adsorption and dissociation that take place on the low Miller index surfaces (i.e., Rh(111), (100), and (110)) and also on polycrystalline Rh. − However, more recent work has focused on the more highly stepped surfaces in an attempt to determine if these surfaces are more active for NO dissociation than flat surfaces. − …”

Section: Introductionmentioning

confidence: 99%

NO Adsorption and Dissociation on Rh(111): PM-IRAS Study

et al. 2006

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We have used in situ polarization-modulation infrared reflection absorption spectroscopy to study the adsorption/dissociation of NO on Rh(111). While these studies have not been conclusive regarding the detailed surface structures formed during adsorption, they have provided important new information on the dissociation of NO on Rh(111). At moderate pressures (< or =10(-6) Torr) and temperatures (<275 K), a transition from 3-fold hollow to atop bonding is apparent. Data indicate that this transition is not due to the migration of the 3-fold hollow NO but rather to the adsorption of gas-phase NO that is directed toward the atop position due to the presence of NO decomposition products, particularly chemisorbed atomic O species at the hollow sites. These results indicate that NO dissociation occurs at temperatures well below the temperature previously reported. Additionally, high pressure (1 Torr) NO exposure at 300 K results in only atop NO, calling into question the surface structures previously proposed at these adsorption conditions consisting of atop and 3-fold hollow sites.

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The interaction of NO with stepped Rh surfaces

Cited by 28 publications

References 63 publications

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

NO Reduction by H₂ on the Rh(111) and Rh(221) Surfaces: A Mechanistic and Kinetic Study

NO Adsorption and Dissociation on Rh(111): PM-IRAS Study

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The interaction of NO with stepped Rh surfaces

Cited by 28 publications

References 63 publications

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

Lateral Interactions and Multi-isotherms: Nitrogen Recombination from Rh(111)

NO Reduction by H2 on the Rh(111) and Rh(221) Surfaces: A Mechanistic and Kinetic Study

NO Adsorption and Dissociation on Rh(111): PM-IRAS Study

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NO Reduction by H₂ on the Rh(111) and Rh(221) Surfaces: A Mechanistic and Kinetic Study