Nitric oxide + carbon monoxide on rhodium(111): steady-state rates and adsorbate coverages

Schwartz, Stuart B.; Fisher, Galen B.; Schmidt, L.D.

doi:10.1021/j100313a030

Cited by 79 publications

(35 citation statements)

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“…Due to the scarcity and high price of Rh and Pd noble metals and increasingly stringent standard for NO emission [61][62][63], continuing improvement of noble metal catalysts for the NO-CO reaction and development of substitutes [5,61,[64][65][66].…”

Section: The No-co Reaction On Rh and Pd Catalystsmentioning

confidence: 99%

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

Chuang

Guzmán

2009

Top Catal

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This paper provides an overview of the use of various transient infrared methods to determine the role of infrared observable species in the mechanisms of the NO-CO reaction, heterogeneous ethylene hydroformylation, and photocatalytic oxidation of ethanol. The transient infrared methods with a judicious choice of ways in changing the concentration of reactants and their isotope counterparts produce responses, allowing (i) identification of the spectators, (ii) determination of active adsorbed species, and (iii) verification of kinetic models and their parameters. The method has also been recently extended to monitor infrared absorbance of photogenerated electrons during photocatalysis, correlating variation in the concentration of photogenerated electrons and adsorbed species. The specific discussion focuses on limitations of the approaches and the type of mechanistic information that can be obtained.

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Section: The No-co Reaction On Rh and Pd Catalystsmentioning

confidence: 99%

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

Chuang

Guzmán

2009

Top Catal

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“…In the reaction of NO reduction by CO in an oxygen excess condition, NO might preferentially adsorbed on the metallic Au clusters where it was dissociated to yield adsorbed N* and O* intermediates, similar to the cases of Pt and Rh as catalyst active phases [16][17][18][19]. The ability of Au to dissociate the adsorbed NO-Au, from an electronic point of view, might be resulted from the d-electrons from 5d atomic orbital in Au atoms back-donation to the 2π*antibonding orbital of adsorbed NO molecule, that activates the NO-Au complex and weakens inlet mixture, the adsorbed O* species originate from the NO dissociation or the surface lattice oxygen of TiO 2 ; however, in the case of oxygen presence in the reaction mixture, the molecular O 2 may be dissociated on the active sites to produce O* species, which may inhibit the NO dissociation, resulting in NO conversion less than 53 % at 200 ºC and 61 % at 400 ºC in the present experiment.…”

Section: Resultsmentioning

confidence: 84%

NO Reduction by CO Catalyzed with Au/TiO₂ in Oxygen-rich Condition

et al. 2010

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Gold nanoparticles supported on titania catalysts with different Au loadings were prepared and evaluated in the reaction of NO reduction by CO in an oxygen rich condition. The crystalline structures of the Au/TiO 2 materials were refined with Rietveld method. TiO 2 support chiefly contains anatase phase, having a crystalline size ranged from 5 to 15 nm. Au particles have an average crystal size approximately 2-5 nm as Au concentration less 3 wt %. In the reaction of NO + CO + O 2 , the Au/TiO 2 catalysts show a selectivity to 100 % N 2 , neither NO 2 nor N 2 O was yielded in the reaction temperature between 25 and 400 ºC, which strongly indicates that Au/TiO 2 catalysts are much superior to the other catalysts like Pt/TiO 2 catalysts on which N 2 O was usually produced in the reaction temperature below 200 °C and NO 2 was produced in the reaction temperature above 300 °C under a similar reaction condition.

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“…NO dissociation is of great importance in NO–CO reaction. Schwartz et al showed that at low temperatures (below 125–175 °C) high NO coverage inhibited NO decomposition. As the temperature increases, NO desorption becomes fast enough to further allow NO to adsorb onto a vacant rhodium site, and NO begins to dissociate.…”

Section: Surface Reaction Mechanismmentioning

confidence: 99%

Detailed kinetic modelling of automotive exhaust NO_x reduction over rhodium catalyst

Xie

et al. 2014

Can J Chem Eng

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The reduction of NO with CO and H2 as the reductants was investigated on the rhodium‐based catalyst over a temperature range of 150–400 °C. Micro‐kinetic modelling method was utilized to compare the activities of CO and H2. Quasi‐elementary mechanisms of NO‐CO and NO‐H2 consisting of 11 and 25 steps, respectively, were proposed. The reaction steps and kinetic parameters were derived from literature and some parameters were optimized to fit the experimental data. Furthermore, to verify the validity range of the developed mechanism, the reaction intermediate N2O reduction by CO and by H2 over Rh were investigated. Over a wide range of reaction conditions, the detailed mechanism predicted experimental results quite well for both NO and N2O conversions with CO and/or H2 as reductant. The phenomenon that NO‐CO and NO‐H2 reactions commenced at similar temperature can be interpreted by the hindered H2 dissociative adsorption steps by extensive NO adsorption. Reaction profiles such as fractional coverages, reaction pathway and sensitivity analysis provided valuable insight into the reaction systems. N2O plays a crucial role in N2 formation for both NO‐CO and NO‐H2 reaction systems. The routes involving N2O formation and decomposition were identified as the dominant pathway in N2 formation at low temperatures.

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Nitric oxide + carbon monoxide on rhodium(111): steady-state rates and adsorbate coverages

Cited by 79 publications

References 0 publications

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

NO Reduction by CO Catalyzed with Au/TiO₂ in Oxygen-rich Condition

Detailed kinetic modelling of automotive exhaust NO_x reduction over rhodium catalyst

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Nitric oxide + carbon monoxide on rhodium(111): steady-state rates and adsorbate coverages

Cited by 79 publications

References 0 publications

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

Mechanistic Investigation of Heterogeneous Catalysis by Transient Infrared Methods

NO Reduction by CO Catalyzed with Au/TiO2 in Oxygen-rich Condition

Detailed kinetic modelling of automotive exhaust NOx reduction over rhodium catalyst

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Product

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NO Reduction by CO Catalyzed with Au/TiO₂ in Oxygen-rich Condition

Detailed kinetic modelling of automotive exhaust NO_x reduction over rhodium catalyst