Experimental measurements and kinetic modeling of CO/H2/O2/NOx conversion at high pressure

Rasmussen, Christian Lund; Hansen, Jens Aage; Marshall, Paul; Glarborg, Peter

doi:10.1002/kin.20327

Cited by 184 publications

(216 citation statements)

References 178 publications

(254 reference statements)

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“…The simulations range from the mixing point for NO and O 2 prior to the reactor to the pressure reduction valve after the reactor where the pressure is reduced to atmospheric level. The entire temperature profile used as model input, based on measurements from [11], is shown in Fig. 1.…”

Section: Resultsmentioning

confidence: 99%

“…The installation is described in detail elsewhere [1,11] and only a brief description is provided here.…”

Section: Methodsmentioning

confidence: 99%

“…The mechanism used for the modeling study, as well as the corresponding thermodynamic properties, was drawn from previous high-pressure work on conversion of CO/H 2 /O 2 /NO x [11], CH 4 /C 2 H 6 /O 2 [12], and CH 4 /O 2 /NO x [13]. Recently, it was updated to describe C 2 H 4 oxidation at high pressure, with particular emphasis on a number of oxygenated C 2 -species important under low-temperature conditions [1].…”

Section: Chemical Kinetic Modelmentioning

confidence: 99%

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High pressure oxidation of C2H4/NO mixtures

Giménez-López

Alzueta

Rasmussen

et al. 2011

Proceedings of the Combustion Institute

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An experimental and kinetic modeling study of the interaction between C 2 H 4 and NO has been performed under flow reactor conditions in the intermediate temperature range (600-900 K), high pressure (60 bar), and for stoichiometries ranging from reducing to oxidizing conditions. The main reaction pathways of the C 2 H 4 /O 2 /NO x conversion, the capacity of C 2 H 4 to remove NO, and the influence of the presence of NO x on the C 2 H 4 oxidation are analyzed. Compared to the C 2 H 4 /O 2 system, the presence of NO x shifts the onset of reaction 75-150 K to lower temperatures. The mechanism of sensitization involves the reaction HOCH 2 CH 2 OO + NO → CH 2 OH + CH 2 O + NO 2 , which pushes a complex system of partial equilibria towards products. This is a confirmation of the findings of Doughty et al. [Proc. Combust. Inst. 26 (1996) 589-596] for a similar system at atmospheric pressure. Under reducing conditions and temperatures above 700 K, a significant fraction of the NO x is removed. This removal is partly explained by the reaction C 2 H 3 + NO → HCN + CH 2 O. However, a second removal mechanism is active in the 700-850 K range, which is not captured by the chemical kinetic model. With the present thermochemistry and kinetics, neither formation of nitro-hydrocarbons

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Section: Resultsmentioning

confidence: 99%

“…The installation is described in detail elsewhere [1,11] and only a brief description is provided here.…”

Section: Methodsmentioning

confidence: 99%

Section: Chemical Kinetic Modelmentioning

confidence: 99%

See 1 more Smart Citation

High pressure oxidation of C2H4/NO mixtures

Giménez-López

Alzueta

Rasmussen

et al. 2011

Proceedings of the Combustion Institute

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“…In the present study, the starting mechanism and corresponding thermodynamic properties were drawn from recent work by the authors on oxidation of H 2 , CO and C 1 /C 2 hydrocarbons [27][28][29][30]. Both the thermochemistry and the HOCHO oxidation subset of the mechanism were carefully updated.…”

Section: Detailed Kinetic Modelmentioning

confidence: 99%

Ab initio and kinetic modeling studies of formic acid oxidation

Marshall

Glarborg

2015

Proceedings of the Combustion Institute

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“…The oxidation pathways for C 2 H 4 under these conditions are different from those prevailing at higher temperatures and lower pressures and the results of the current work help to extend the validation range for chemical kinetic modeling of C 2 H 4 oxidation. This paper is part of a series investigating the high-pressure, medium temperature oxidation of simple fuels: previously work has been reported for CO/H 2 , CH 4 , and CH 4 /C 2 H 6 mixtures [18,19]. The present kinetic model draws on this work, as well as recent results in tropospheric chemistry.…”

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confidence: 94%

Experimental and kinetic modeling study of C2H4 oxidation at high pressure

López

Rasmussen

Alzueta

et al. 2009

Proceedings of the Combustion Institute

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A detailed chemical kinetic model for oxidation of C 2 H 4 in the intermediate temperature range and high pressure has been developed and validated experimentally. New ab initio calculations and RRKM analysis of the important C 2 H 3 + O 2 reaction was was used to obtain rate coefficients over a wide range of conditions (0.003-100 bar, 200-3000 K). The results indicate that at 60 bar vinyl peroxide, rather than CH 2 O and HCO, is the dominant product.The experiments, involving C 2 H 4 /O 2 mixtures diluted in N 2 , were carried out in a high pressure flow reactor at 600-900 K and 60 bar, varying the reaction stoichiometry from very lean to fuel-rich conditions. Model predictions are generally satisfactory. The governing reaction mechanisms are outlined based on calculations with the kinetic model. Under the investigated conditions the oxidation pathways for C 2 H 4 are more complex than those prevailing at higher temperatures and lower pressures. The major differences are the importance of the hydroxyethyl (CH 2 CH 2 OH) and 2-hydroperoxyethyl 1 (CH 2 CH 2 OOH) radicals, formed from addition of OH and HO 2 to C 2 H 4 , and vinyl peroxide, formed from C 2 H 3 + O 2 . Hydroxyethyl is oxidized through the peroxide HOCH 2 CH 2 OO (lean conditions) or through ethenol (low O 2 concentration), while 2-hydroperoxyethyl is converted through oxirane. [2][3][4][5][6][7], shock tubes [8][9][10][11][12] and premixed laminar flames [13][14][15][16][17], covering a wide range of stoichiometries and temperatures. Most of the reported work, however, have been carried out at near atmospheric pressure. A few results are available from flow reactor studies at 5-10 bar [6], but despite their relevance for the chemistry in engines, gas turbines, and gas-to-liquid processes, data at high pressures are limited.The objective of the present study is to obtain experimental results for the oxidation of C 2 H 4 at high pressure (60 bar) as functions of temperature (600-900 K) and stoichiometry (lean to fuel-rich) and analyze them in terms of a detailed chemical kinetic model. The oxidation pathways for C 2 H 4 under these conditions are different from those prevailing at higher temperatures and lower pressures and the results of the current work help to extend the validation range for chemical kinetic modeling of C 2 H 4 oxidation. This paper is part of a series investigating the high-pressure, medium temperature oxidation of simple fuels: previously work has been reported for CO/H 2 , CH 4 , and CH 4 /C 2 H 6 mixtures [18,19]. The present kinetic model draws on this work, as well as recent results in tropospheric chemistry. Furthermore, the important reaction of C 2 H 3 with O 2 was characterized from ab initio calculations over a wide range of pressure and temperature. 3 ExperimentalThe experimental setup is a laboratory-scale high pressure laminar flow reactor designed to approximate plug-flow. The setup is described in detail elsewhere [18] and only a brief description is provided here. The system enables well-defined investigations of...

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Experimental measurements and kinetic modeling of CO/H₂/O₂/NO_x conversion at high pressure

Cited by 184 publications

References 178 publications

High pressure oxidation of C2H4/NO mixtures

High pressure oxidation of C2H4/NO mixtures

Ab initio and kinetic modeling studies of formic acid oxidation

Experimental and kinetic modeling study of C2H4 oxidation at high pressure

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