Kinetics of ammonia-nitric oxide reactions on vanadium oxide catalysts

Farber, Milton; Harris, Sigmund P.

doi:10.1021/j150648a013

Cited by 42 publications

(17 citation statements)

References 3 publications

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“…We have proposed a possible reaction mechanism for both the formation of the H 2 NNO species and its subsequent dissociation into H 2 O and N 2 (Scheme 1). This mechanism is consistent with results that H 2 NNO is viable within clusters with a lifetime in the microsecond regime [44,45]. The H 2 NNO cluster ion may then be either stabilized (via cluster solvation) or dissociate to generate H 2 O plus N 2 , where the water is then retained within the cluster.…”

Section: Resultssupporting

confidence: 89%

“…The formation of H 2 NNO and its relevant chemical reactions have become a subject of tremendous studies, both theoretically [49][50][51][52][53] and experimentally [54][55][56][57]. A substantial fraction of the work has been centered mainly on the kinetic and energetic aspects for the reaction between NH 2 and NO, leading to the formation of [44,45,58]. The H 2 NNO species was observed during the catalytic chemical reaction of NH 3 and NO gas mixtures on vanadium oxide catalysts via mass spectrometry [44].…”

Section: Discussionmentioning

confidence: 99%

“…A substantial fraction of the work has been centered mainly on the kinetic and energetic aspects for the reaction between NH 2 and NO, leading to the formation of [44,45,58]. The H 2 NNO species was observed during the catalytic chemical reaction of NH 3 and NO gas mixtures on vanadium oxide catalysts via mass spectrometry [44]. Matrix infrared study [58] (and ab initio calculation) led to identification of H 2 NNO, where the low temperature would prevent rapid dissociation of the H 2 NNO species.…”

Section: Discussionmentioning

confidence: 99%

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Nitrosamide, (H2NNO), formation within [(NO)m(NH3)n]+ clusters: Theory and experiment

Shin

Freindorf

Furlani

et al. 2006

International Journal of Mass Spectrometry

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Section: Resultssupporting

confidence: 89%

Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

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Nitrosamide, (H2NNO), formation within [(NO)m(NH3)n]+ clusters: Theory and experiment

Shin

Freindorf

Furlani

et al. 2006

International Journal of Mass Spectrometry

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“…9 This is supported by mass spectroscopic data that indicate the presence of NH 2 NO during the reaction of NH 3 with NO on vanadium oxide catalysts. 16 Moreover, NH 2 NO was identified as intermediate in most of the theoretical studies of the SCR reaction at clean as well as at TiO 2 supported V 2 O 5 surfaces. [17][18][19][20][21] Further, theoretical studies showed that the reaction of NO with NH 2 in gas phase proceeds via the NH 2 NO intermediate.…”

Section: Introductionmentioning

confidence: 99%

Elementary steps of the catalytic NOx reduction with NH3: Cluster studies on reactant adsorption at vanadium oxide substrate

Gruber

Hermann

2013

The Journal of Chemical Physics

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Extended cluster models together with density-functional theory are used to evaluate geometric, energetic, and electronic properties of different adsorbate species that can occur at a vanadium oxide surface where the selective catalytic reduction (SCR) of NO in the presence of ammonia proceeds. Here, we focus on atomic hydrogen, nitrogen, and oxygen, as well as molecular NO and NHx, x = 1, 4, adsorption at a model V2O5(010) surface. Binding sites, oxygen and vanadium, at both the perfect and reduced surface are considered where reduction is modeled by (sub-) surface oxygen vacancies. The reactants are found to bind overall more strongly at oxygen vacancy sites of the reduced surface where they stabilize in positions formerly occupied by the oxygen (substitutional adsorption) compared with weaker binding at the perfect surface. In particular, ammonia, which interacts only weakly with vanadium at the perfect surface, binds quite strongly near surface oxygen vacancies. In contrast, surface binding of the NH4 adsorbate species differs only little between the perfect and the reduced surface which is explained by the dominantly electrostatic nature of the adsorbate interaction. The theoretical results are consistent with experimental findings and confirm the importance of surface reduction for the reactant adsorption forming elementary steps of the SCR process.

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“…Currently, the reaction is regarded by most workers in the field as an Eley-Rideal mechanism, where ammonia adsorbs onto the surface and where NO reacts from the gas phase or as weakly adsorbed species on the surface [30][31][32][33][34][35][36]. Most adsorption experiments show very weak signs of adsorption of NO on the surface.…”

Section: Scr Reaction Mechanism For Vanadium Catalysts: the Eley-ridementioning

confidence: 99%

Flue Gases from Stationary Sources

Gabrielsson

Pedersen

2008

Handbook of Heterogeneous Catalysis

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The sections in this article are Emissions from Stationary Sources Drivers for Flue Gas Cleaning Technology The USA E urope A sia C hina J apan NO x Removal Technologies Nitrous Oxide (N 2 O) Selective Catalytic Reduction ( SCR ) SCR Technology SCR Catalysts Different Catalyst Types Choice of Carrier Optimization of Activity The Effect of Increasing V 2 O 5 Loading Activation Energy as a Function of Vanadium Content The Effect of Co‐Oxides SCR Reaction Mechanism for Vanadium Catalysts: the Eley–Rideal Route Global Kinetics The Importance of B rønsted Acidity The Influence of Reoxidation or NO 2 The Influence of Gas Composition on Reaction Rate The Influence of Water The Influence of O 2 Modeling Definition of Different Model Types Estimation of Interphase Mass Transfer Intraporous Mass Transfer Kinetic Expressions The Feasibility of Different Models Deactivation Chemical Poisoning Surface Fouling, Pore and Channel Clogging Sintering Catalyst Management and Regeneration SCR Catalyst Testing Laboratory‐ and Bench‐Scale Testing Pilot‐Scale Testing Slip‐Stream Reactors Full‐Scale Catalyst Testing Gas Sampling and Analysis Other Emissions Sulfur Removal The Wet Sulfuric Acid ( WSA ) Process and Combined WSA and De NO x ( SNOX ) Hydrogen Sulfide Carbon Monoxide Carbon Dioxide Hydrocarbons Dioxins Hg Oxidation and Capture Hg Oxidation Thermodynamics Hg Removal from Coal‐Fired Power Plants A Conventional Flue Gas Cleaning Processes B Sorbent Injection, Coal Additives, and Coal Blending Hg Oxidation Mechanism and Catalysis Alternative Processes Multipollutant Processes The DESONOX Process Other Combined Processes Catalytic Filters New Technologies Plasma‐Assisted Processes Photocatalytic Processes

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Kinetics of ammonia-nitric oxide reactions on vanadium oxide catalysts

Cited by 42 publications

References 3 publications

Nitrosamide, (H2NNO), formation within [(NO)m(NH3)n]+ clusters: Theory and experiment

Nitrosamide, (H2NNO), formation within [(NO)m(NH3)n]+ clusters: Theory and experiment

Elementary steps of the catalytic NOx reduction with NH3: Cluster studies on reactant adsorption at vanadium oxide substrate

Flue Gases from Stationary Sources

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