Experimental and kinetic modeling study of the effect of NO and SO<sub>2</sub> on the oxidation of COH<sub>2</sub> mixtures

Dagaut, Philippe; Lecomte, Franck; Mieritz, Jacob; Glarborg, Peter

doi:10.1002/kin.10154

Cited by 88 publications

(102 citation statements)

References 38 publications

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“…7,[10][11][12]16,17 In addition to k 1 , k 2 , and k 3 , only one rate constant has been modified in the present work. For the SO 2 + SO 2 reaction (6), we use an estimate, based on batch reactor results on SO 2 + O 2 , 31 discussed below, and shock tube results on SO 2 decomposition.…”

Section: Detailed Kinetic Modelmentioning

confidence: 99%

“…18,19,23 In conflict with these results, Alzueta et al 10 recommend a very low rate constant, which indicates that the reaction is insignificant under most conditions of interest. In the absence of measurements, the SO 3 + OH reaction (3) has been omitted from most previous modeling studies of sulfur chemistry, 7,10,[14][15][16] but it is potentially an important step.…”

Section: Introductionmentioning

confidence: 99%

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Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions

Hindiyarti

Glarborg²,

Marshall

2007

J. Phys. Chem. A

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The reactions of SO 3 with H, O, and OH radicals have been investigated by ab initio calculations. For the SO 3 + H reaction (1), the lowest energy pathway involves initial formation of HSO 3 and rearrangement to HOSO 2 , followed by dissociation to OH + SO 2 . The reaction is fast, with k 1 ) 8.4 × 10 9 T 1.22 exp(-13.9 kJ mol -1 /RT) cm 3 mol -1 s -1 (700-2000 K). The SO 3 + O f SO 2 + O 2 reaction (2) may proceed on both the triplet and singlet surfaces, but due to a high barrier the reaction is predicted to be slow. The rate constant can be described as k 2 ) 2.8 × 10 4 T 2.57 exp(-122.3 kJ mol -1 /RT) cm 3 mol -1 s -1 for T > 1000 K. The SO 3 + OH reaction to form SO 2 + HO 2 (3) proceeds by direct abstraction but is comparatively slow, with k 3 ) 4.8 × 10 4 T 2.46 exp(-114.1 kJ mol -1 /RT) cm 3 mol -1 s -1 (800-2000 K). The revised rate constants and detailed reaction mechanism are consistent with experimental data from batch reactors, flow reactors, and laminar flames on oxidation of SO 2 to SO 3 . The SO 3 + O reaction is found to be insignificant during most conditions of interest; even in lean flames, SO 3 + H is the major consumption reaction for SO 3 .

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Section: Detailed Kinetic Modelmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions

Hindiyarti

Glarborg²,

Marshall

2007

J. Phys. Chem. A

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“…18). Comparable agreement is achieved for the flow reactor experiment of Dagaut et al [64]. The different optimized versions lead to slight variations of the predicted profiles for the case with SO 2 , but the overall quality of the prediction is not altered significantly.…”

Section: Validation: Interactions Between Ch 4 and H 2 Smentioning

confidence: 60%

“…One possible interaction between carbon and sulfur species is the inhibition of CO oxidation by SO 2 [30,31,63,64]. The combined mechanism can capture the inhibiting effect of SO 2 on CO oxidation at stoichiometric conditions observed by Giménez-López et al [63] both in a nitrogen (N 2 ) bath and in the presence of CO 2 (see Fig.…”

Section: Validation: Interactions Between Ch 4 and H 2 Smentioning

confidence: 90%

Chemical kinetics mechanism for oxy-fuel combustion of mixtures of hydrogen sulfide and methane

Bongartz

Ghoniem

2015

Combustion and Flame

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Oxy-fuel combustion of sour gas, a mixture of natural gas (essentially methane (CH 4 )), carbon dioxide (CO 2 ), and hydrogen sulfide (H 2 S), could enable the utilization of large natural gas resources, especially when combined with enhanced oil recovery. In this work, a detailed chemical reaction mechanism for oxy-fuel combustion of sour gas is presented. To construct the mechanism, a CH 4 sub-mechanism was chosen based on a comparative validation study for oxy-fuel combustion. This mechanism was combined with a mechanism for H 2 S oxidation, and the sulfur sub-mechanism was then optimized to give better agreement with relevant experiments. The optimization targets included predictions for the laminar burning velocity, ignition delay time, and pyrolysis of H 2 S, and H 2 S oxidation in a flow reactor. The rate parameters of 15 sulfur reactions were varied in the optimization within their respective uncertainties. The optimized combined mechanism was validated against a larger set of experimental data over a wide range of conditions for oxidation of H 2 S and interactions between carbon and sulfur species. Improved overall agreement was achieved through the optimization and all important trends were captured in the modeling results. The optimized mechanism can be used to make qualitative and some quantitative predictions on the combustion behavior of sour gas. The remaining discrepancies highlight the current uncertainties in sulfur chemistry and underline the need for more accurate direct determination of several important rate constants as well as more validation data.

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“…For example, Glarborg et al [94], investigated the reaction of ammonia with NO 2 through a flow reactor and detailed reaction kinetics, Bromly et al [95], examined effects of NO on oxidation of H 2 , and Dagaut et al [96], studied effects of NO and SO 2 on oxidation of CO-H 2 mixtures. Recently, Smith et al [97], have proposed new schemes that need not be used because the gasified fuel contains a small percent of CH 4 and no C 2 hydrocarbon.…”

Section: Supplied Fuels and Test Conditionsmentioning

confidence: 99%

Gas Turbine Combustion and Ammonia Removal Technology of Gasified Fuels

Hasegawa

2010

Energies

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From the viewpoints of securing a stable supply of energy and protecting our global environment in the future, the integrated gasification combined cycle (IGCC) power generation of various gasifying methods has been introduced in the world. Gasified fuels are chiefly characterized by the gasifying agents and the synthetic gas cleanup methods and can be divided into four types. The calorific value of the gasified fuel varies according to the gasifying agents and feedstocks of various resources, and ammonia originating from nitrogenous compounds in the feedstocks depends on the synthetic gas clean-up methods. In particular, air-blown gasified fuels provide low calorific fuel of 4 MJ/m 3 and it is necessary to stabilize combustion. In contrast, the flame temperature of oxygen-blown gasified fuel of medium calorie between approximately 9-13 MJ/m 3 is much higher, so control of thermal-NOx emissions is necessary. Moreover, to improve the thermal efficiency of IGCC, hot/dry type synthetic gas clean-up is needed. However, ammonia in the fuel is not removed and is supplied into the gas turbine where fuel-NOx is formed in the combustor. For these reasons, suitable combustion technology for each gasified fuel is important. This paper outlines combustion technologies and combustor designs of the high temperature gas turbine for various IGCCs. Additionally, this paper confirms that further decreases in fuel-NOx emissions can be achieved by removing ammonia from gasified fuels through the application of selective, non-catalytic denitration. From these basic considerations, the performance of specifically designed combustors for each IGCC proved the proposed methods to be sufficiently effective. The combustors were able to achieve strong results, decreasing thermal-NOx emissions to 10 ppm (corrected at 16% oxygen) or less, and fuel-NOx emissions by 60% or more, under conditions where ammonia concentration per fuel heating value in unit volume was 2.4 × 10 2 ppm/(MJ/m 3 ) or higher. Average equivalence ratio at combustor exhaust φ p Average equivalence ratio in primary combustion zone ΔP/q Total pressure loss coefficient (characteristic section is combustor-exit) OPEN ACCESS

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Experimental and kinetic modeling study of the effect of NO and SO₂ on the oxidation of COH₂ mixtures

Cited by 88 publications

References 38 publications

Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions

Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions

Chemical kinetics mechanism for oxy-fuel combustion of mixtures of hydrogen sulfide and methane

Gas Turbine Combustion and Ammonia Removal Technology of Gasified Fuels

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Experimental and kinetic modeling study of the effect of NO and SO2 on the oxidation of COH2 mixtures

Cited by 88 publications

References 38 publications

Reactions of SO3 with the O/H Radical Pool under Combustion Conditions

Reactions of SO3 with the O/H Radical Pool under Combustion Conditions

Chemical kinetics mechanism for oxy-fuel combustion of mixtures of hydrogen sulfide and methane

Gas Turbine Combustion and Ammonia Removal Technology of Gasified Fuels

Contact Info

Product

Resources

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Experimental and kinetic modeling study of the effect of NO and SO₂ on the oxidation of COH₂ mixtures

Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions

Reactions of SO₃ with the O/H Radical Pool under Combustion Conditions