The Rate and Mechanism of the Air Oxidation of Parts-per-Million Concentrations of Nitric Oxide in the Presence of Water Vapor

England, C.; Corcoran, W. H.

doi:10.1021/i160053a010

Cited by 38 publications

(22 citation statements)

References 15 publications

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“…In Equation (2), r NO represents the rate of nitric oxide oxidation. The majority of the published papers 1–21 are in agreement with Equation (2). The data obtained by these authors on the rate constant k 1 are summarized in Table 1.…”

Section: Literature Reviewsupporting

confidence: 63%

Kinetic study of the nitric oxide oxidation between 288 and 323 K, under pressure, focus on the oxygen influence on the reaction rate constant

Neyrolles

Cruz

Bassil

et al. 2020

Int J of Chemical Kinetics

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The sequestration of carbon dioxide fumes from oxyfuel combustion is used to reduce significantly the carbon dioxide emissions from coal‐fired power plants. Impurities like nitric oxide, present in the fumes, can cause technical difficulties during the capture, the treatment, the transport, and the storage steps of the CO2 fumes. The purpose of this study is to better understand the oxidation of nitric oxide under pressure in the presence of carbon dioxide and in the experimental condition of flue gas treatment. This reaction is known to be a third‐order reaction, two order in nitric oxide and first order in oxygen. To examine the effect of the temperature, the pressure and the volume fraction of oxygen on the rate constant of oxidation, k1, an autoclave is used. The first experiment studies the influence of the temperature between 288 and 323 K. The results found are in the form of an Arrhenius‐type equation: k1 = 810 exp(620/T) and are in agreement with the literature. Carbon dioxide does not seem to have an influence on the rate constant, whereas our experimental measurements indicate an influence of the volume fraction of oxygen. The rate constant decreases when the oxygen volume fraction increases by up to 10%. Then the rate constant remains constant. This observation allows us to conclude that the mechanism involving the mechanism with a dimer of NO as an intermediate is more likely to be the mechanism involved in the nitric oxide oxidation in our experimental conditions: high pressure and ambient temperature. The rate constant k2, k–2, and k3 were also estimated in these conditions.

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Section: Literature Reviewsupporting

confidence: 63%

Kinetic study of the nitric oxide oxidation between 288 and 323 K, under pressure, focus on the oxygen influence on the reaction rate constant

Neyrolles

Cruz

Bassil

et al. 2020

Int J of Chemical Kinetics

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show abstract

“…These reactions correspond to relatively well established rate processes. The most uncertain rate constant corresponds to NO oxidation at the interface which was estimated using the data of England and Corcoran [54]. These authors observed that the heterogeneous feature of the NO oxidation was not reproducible and the rate constant for reaction (1b) must be taken with caution due to the large uncertainty of the experimental data.…”

Section: The Proposed Model For N 2 O Formationmentioning

confidence: 99%

The heterogeneous formation of N2O in the presence of acidic solutions: Experiments and modeling

Pires¹,

Rossi²

1997

Int. J. Chem. Kinet.

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We investigated the heterogeneous processes that contribute towards the formation of N 2 O in an environment that comes as closely as possible to exhaust conditions containing NO and SO 2 among other constituents. The simultaneous presence of NO, SO 2 , O 2 , and condensed phase water in the liquid state has been confirmed to be necessary for the production of significant levels of N 2 O. The maximum rate of N 2 O formation occurred at the beginning of the reaction and scales with the surface area of the condensed phase and is independent of its volume. The replacement of NO by either NO 2 or HONO significantly increases the rate constant for N 2 O formation. The measured reaction orders in the rate law change depending upon the choice of the nitrogen reactant used and were fractional in some cases. The rate constants of N 2 O formation for the three different nitrogen reactants reveal the following series of increasing reactivity:indicating the probable se-NO Ͻ NO Ͻ HONO, 2 quential involvement of those species in the elementary reactions. Furthermore, we observed a complex dependence of the rate constant on the acidity of the liquid phase where both the initial rate as well as the yield of N 2 O are largest at of a H 2 SO 4 /H 2 O solution. The pH ϭ 0 results suggest that HONO is the major reacting N(III) species over a wide range of acidities studied. The N 2 O formation in synthetic flue gas may be simulated using a relatively simple mechanism based on the model of Lyon and Cole. The first step of the complex overall reaction corresponds to NO oxidation by O 2 to NO 2 mainly in the gas phase, with the presence of both H 2 O and active surfaces significantly accelerating NO 2 production. Subsequently, NO 2 reacts with excess NO to obtain HONO which reacts with S(IV) to result in N 2 O and H 2 SO 4 through a complex reaction sequence probably involving nitroxyl (HON) and its dimer, hyponitrous acid.

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“…Reaction 1 proceeds at a rate which is proportional to the square of the NO concentration and which decreases as temperature is increased. Some estimates are available for the rate of reaction 5 (England and Corcoran, 1975) and the equilibrium constant can be calculated. When the NO partial pressure is comparable to or greater than that of NO2, the equilibrium concentration of nitric acid is very small for typical process conditions.…”

Section: Nitrogen Oxide Chemistrymentioning

confidence: 99%

“…In this work it was theorized that, with a sufficiently fast rate of formation of HNO,, the gas phase limited mass transfer of HNO, could be enhanced by formation of HNO, in the gas film. If one uses the kinetic data of England and Corcoran (1975) and the data of Corriveau (1971) for the absorption of N,O, in water, enhancement can be shown to occur a t high partial pressures of NO, with the gas-side coefficients typically found in gas absorption towers.…”

Section: Absorption Of Nitrogen Oxides In Aqueous Solutionsmentioning

confidence: 99%

Mass transfer in the absorption of nitrogen oxides in alkaline solutions

Newman

Carta

1988

AIChE Journal

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The absorption of mixtures of nitrogen oxides into aqueous solutions of NaOH in the range of partial pressures of 0.004-to O.05-atm NO and 0.002-to 0.015-atm NO, was investigated. Absorption experiments were conducted in a gas-liquid contactor that permitted independent variation of the gas and liquid mass transfer coefficients. The results were analyzed in terms of a model which accounted for diffusion, reaction, and formation of higher oxides and oxyacids in the gas and in the liquid phases. Absorption of both HNO, and N,03, formed in the bulk gas and within the gas diffusion film, were found to be significant. Using a rate coefficient of 8.8 x lop3 mol/s -cm3 -atm3 for the formation of HNO, in the gas phase (England and Corcoran, 1975) a value of the absorption factor, H c k , for N,03 of 2.5 x mol/s cm2 atm was determined at 25°C. This value was found to decrease with temperature and was 1.2 x at 40°C. The use of concentrated base as an absorbent solution prevented the formation of nitric acid mist, a problem encountered in many previous studies of NO, absorption.

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The Rate and Mechanism of the Air Oxidation of Parts-per-Million Concentrations of Nitric Oxide in the Presence of Water Vapor

Cited by 38 publications

References 15 publications

Kinetic study of the nitric oxide oxidation between 288 and 323 K, under pressure, focus on the oxygen influence on the reaction rate constant

Kinetic study of the nitric oxide oxidation between 288 and 323 K, under pressure, focus on the oxygen influence on the reaction rate constant

The heterogeneous formation of N2O in the presence of acidic solutions: Experiments and modeling

Mass transfer in the absorption of nitrogen oxides in alkaline solutions

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