Enhanced SO3 emissions from staged combustion

Merryman, E.L.; Levy, A.

doi:10.1016/s0082-0784(79)80071-5

Cited by 14 publications

(37 citation statements)

References 7 publications

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“…The latter include the room-temperature result of Atkinson and Pitts, Jr. 8 and indirect measurements by Merryman and Levy from flames. 14 The results from the flow reactor study of Mueller et al 7 and the shock tube study of Hwang et al 15 on the reaction are not included, since they were obtained at higher pressures. The hightemperature data of Astholz et al 10 and Smith et al 12 are shown, even though they relate to argon as a bath gas.…”

Section: Resultsmentioning

confidence: 99%

“…4,5 Flow reactor studies of SO 2 oxidation under post-flame conditions 5,7 indicate fractional conversions of SO 2 to SO 3 of the order of a few percent. According to these studies, SO 3 formation occurs primarily through the reaction Direct measurements are available for this reaction in the 300-800 K range 8,9 and for the reverse reaction, thermal dissociation of SO 3 , in the temperature range of 1700-2500 K. 10 Indirect determinations are available from flames [12][13][14] and shock tube experiments. 15 The rate constant increases with temperature at lower temperatures, peaks at around 750 K, and drops off as the temperature increases further.…”

Section: Introductionmentioning

confidence: 99%

“…In addition, the more accurate value available for k 1 allows for a reassessment of the rate constant for the reaction SO 3 + O f SO 2 + O 2 (R2) obtained from flame measurements. [12][13][14] …”

Section: Introductionmentioning

confidence: 99%

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Thermal Dissociation of SO₃ at 1000−1400 K

et al. 2006

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The thermal dissociation of SO 3 has been studied for the first time in the 1000-1400 K range. The experiments were conducted in a laminar flow reactor at atmospheric pressure, with nitrogen as the bath gas. On the basis of the flow reactor data, a rate constant for SO 3 + N 2 f SO 2 + O + N 2 (R1b) of 5.7 × 10 17 exp(-40000/T) cm 3 /(mol s) is derived for the temperature range 1273-1348 K. The estimated uncertainty is a factor of 2. The rate constant corresponds to a value of the reverse reaction of k 1 ≈ 1.8 × 10 15 cm 6 mol -2 s -1 . The reaction is in the falloff region under the investigated conditions. The temperature and pressure dependence of SO 2 + O (+N 2 ) was estimated from the extrapolation of low temperature results for the reaction, together with an estimated broadening parameter and the high-pressure limit determined recently by Naidoo, Goumri, and Marshall (Proc. Combust. Inst. 2005, 30, 1219-1225. The theoretical rate constant is in good agreement with the experimental results. The improved accuracy in k 1 allows a reassessment of the rate constant for SO 3 + O f SO 2 + O 2 (R2) based on the data of Smith, Tseregounis, and Wang (Int. J. Chem. Kinet. 1982, 14, 679-697), who conducted experiments on a low-pressure CO/O 2 /Ar flame doped with SO 2 . At the location in the flame where the net SO 3 formation rate is zero,A value of 6.9 × 10 10 cm 3 mol -1 s -1 is obtained for k 2 at 1269 K with an uncertainty a factor of 3. A recommended rate constant k 2 ) 7.8 × 10 11 exp(-3065/T) cm 3 mol -1 s -1 is consistent with other flame results as well as the present flow reactor data.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Thermal Dissociation of SO₃ at 1000−1400 K

et al. 2006

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“…10,16,17 The rate constant for the reaction between SO 3 and O (2) has not been measured directly and reported data vary by several orders of magnitude. Indirect determinations have been reported on the basis of results from laminar premixed flames [18][19][20][21][22] and, for the reverse step, from reactor experiments. 10,23 A recent re-interpretation of selected flame results, 12 based on a more accurate value of k 4 , indicates a fairly high rate constant for reaction SO 3 + O h SO 2 + O 2 , in agreement with earlier evaluations, [20][21][22] and a fast reaction is also supported by other experiments.…”

Section: Introductionmentioning

confidence: 99%

“…Indirect determinations have been reported on the basis of results from laminar premixed flames [18][19][20][21][22] and, for the reverse step, from reactor experiments. 10,23 A recent re-interpretation of selected flame results, 12 based on a more accurate value of k 4 , indicates a fairly high rate constant for reaction SO 3 + O h SO 2 + O 2 , in agreement with earlier evaluations, [20][21][22] and a fast reaction is also supported by other experiments. 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.…”

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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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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Sulfur trioxide formation/emissions in coal‐fired air‐ and oxy‐fuel combustion processes: a review

et al. 2018

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In oxy‐fuel combustion, fuel is burned using oxygen together with recycled flue gas, which is needed to control the combustion temperature. This leads to higher concentrations of sulfur dioxide and sulfur trioxide in the recycled gas, which can result in the formation of sulfuric acid and enhanced corrosion. Current experimental data on SO3 formation, reaction mechanisms, and mathematical modelling have indicated significant differences in SO3 formation between air‐ and oxy‐fuel combustion for both the wet and dry flue gas recycle options. This paper provides an extensive review of sulfur trioxide formation in air‐ and oxy‐fuel combustion environments, with an emphasis on coal‐fired systems. The first part summarizes recent findings on oxy‐fuel combustion experiments, as they affect sulfur trioxide formation. In the second part, the review focuses on sulfur trioxide formation mechanisms, and the influence of catalysis on sulfur trioxide formation. Finally, the current methods for measuring sulfur trioxide concentration are also reviewed along with the major difficulties associated with those measurements using data available from both bench‐ and pilot‐scale units. © 2018 Society of Chemical Industry and John Wiley & Sons, Ltd.

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Enhanced SO3 emissions from staged combustion

Cited by 14 publications

References 7 publications

Thermal Dissociation of SO₃ at 1000−1400 K

Thermal Dissociation of SO₃ at 1000−1400 K

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

Sulfur trioxide formation/emissions in coal‐fired air‐ and oxy‐fuel combustion processes: a review

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Enhanced SO3 emissions from staged combustion

Cited by 14 publications

References 7 publications

Thermal Dissociation of SO3 at 1000−1400 K

Thermal Dissociation of SO3 at 1000−1400 K

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

Sulfur trioxide formation/emissions in coal‐fired air‐ and oxy‐fuel combustion processes: a review

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Product

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Thermal Dissociation of SO₃ at 1000−1400 K

Thermal Dissociation of SO₃ at 1000−1400 K

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