A kinetic study of the reaction of atomic oxygen with SO2

Naidoo, Jacinth; Goumri, Abdellatif; Marshall, Paul

doi:10.1016/j.proci.2004.08.214

Cited by 34 publications

(52 citation statements)

References 27 publications

(46 reference statements)

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“…The product gas from the homogeneous reactor is analyzed. (4)(5)(6)(7)(8)(9)(10) Step 3 is repeated for temperatures of 948, 973, 998, 1023, 1048, 1073, and 1176 K. , from which k 1b can easily be obtained. Since R2 is comparatively fast according to the flame measurements, the inequality is almost fulfilled and the error in the values in k 1b from the simple analysis, compared to the detailed analysis, is only of the order of 30%.…”

Section: Resultsmentioning

confidence: 99%

“…The value of k 2 is then easily derived Since the concentration of the O atom drops out of the equation, the uncertainty in the value of k 2 is associated with uncertainties in k 1,Ar (adopted from Naidoo et al 9 ) and the measurements of [SO 2 ], [SO 3 ], and flame temperature. We obtain a value of k 2 (1269 K) ) 6.9 × 10 10 cm 3 mol -1 s -1 with an estimated uncertainty of less than a factor 3.…”

Section: Numerical Procedures and Reaction Mechanismmentioning

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%

“…A Rice-Ramsperger-Kassel-Marcus (RRKM) extrapolation of the low-temperature measurements is in good agreement with data for both the forward and backward reaction over a temperature range of 220-2500 K for Ar as collision partner. 9 Even above 1000 K the reaction is in the falloff region at atmospheric pressure. 7,9 Reaction 1 is important not only for the formation of SO 3 in combustion systems but also in some industrial processes.…”

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: Numerical Procedures and Reaction Mechanismmentioning

confidence: 99%

Section: Introductionmentioning

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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“…We set it equal to the value measured for the spin-forbidden O + SO 2 addition, 3.6 × 10 11 cm 3 mol −1 s −1 . 52 This is a crude estimate and might be uncertain perhaps by an order of magnitude. Other singlet CS 2 O 2 species, with five-and three-membered rings, have also been characterized.…”

Section: ■ Detailed Kinetic Modelmentioning

confidence: 99%

Oxidation of Reduced Sulfur Species: Carbon Disulfide

et al. 2014

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A detailed chemical kinetic model for oxidation of CS 2 has been developed, on the basis of ab initio calculations for key reactions, including CS 2 + O 2 and CS + O 2 , and data from literature. The mechanism has been evaluated against experimental results from static reactors, flow reactors, and shock tubes. The CS 2 + O 2 reaction forms OCS + SO, with the lowest energy path involving crossing from the triplet to the singlet surface. For CS + O 2 , which yields OCS + O, we found a high barrier to reaction, causing this step to be important only at elevated temperatures. The model predicts low temperature ignition delays and explosion limits accurately, whereas at higher temperatures it appears to overpredict both the induction time for CS 2 oxidation and the formation rate of [O] upon ignition. The predictive capability of the model depends on the accuracy of the rate constant for the initiation step CS 2 + O 2 , which is difficult to calculate due to the intersystem crossing, and the branching fraction for CS 2 + O, which is measured only at low temperatures. The governing reaction mechanisms are outlined on the basis of calculations with the kinetic model. ■ INTRODUCTIONOff-gases containing carbon disulfide (CS 2 ) are produced together with other sulfur containing compounds such as H 2 S from a range of industrial processes, including the Claus process 1−3 and production of viscous fibers, 4 and in gasification of coal 5 and biomass. 6 Similar to H 2 S and the oxidation product SO 2 , carbon disulfide is toxic and harmful to the environment. Efficient treatment of the sulfur containing off gases becomes a bottleneck in these processes as strict emission requirements must be met. Hence, knowledge of the CS 2 oxidation mechanism is important. Investigations have shown that CS 2 / O 2 mixtures are able to autoignite at low temperature and low pressure 7−13 under conditions of negligible self-heating. Two explosion limits have been reported in the literature, 7−9 and studies have been carried out to determine the effect upon the limits with a change in surface conditions and addition of inert gases. The induction times range from a few seconds to several minutes. 9,11,14 At higher temperatures, CS 2 oxidation has been investigated in flow reactors, 2,15 shock tubes, 16−18 and laminar premixed flames. 19−23 Much of the high-temperature work has been motivated by interest in the CO laser. CS 2 /O 2 flames form CO with its vibrational population inverted, facilitating production of a CO flame laser.Previous studies of the reaction mechanism of carbon disulfide oxidation have mostly been restricted to fuel-lean, dry conditions. 17,18,20,24,25 No reported chemical kinetic models are found to satisfactory describe experimental data across a wider range of mixture composition, temperature, and pressure as the mechanism is complex and accurate kinetic data have been unavailable for several important reactions. The objective of the present study is to develop a detailed chemical kinetic model for oxidation of...

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Thermal Integration of Sulfuric Acid and Continuous Catalyst Regeneration of Naphtha Reforming Plants

et al. 2018

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An optimal reactor design is proposed that simultaneously improves the naphtha reforming reactor performance and increases sulfur trioxide production. In this new configuration, the naphtha reforming process as an endothermic reaction is coupled with the oxidation reaction of sulfur dioxide, which is an exothermic reaction. The differential evolution optimization technique is applied to maximize the produced amounts and yields of aromatics and hydrogen. The results obtained with the optimized thermally coupled reactor are compared with those of the conventional and thermally coupled reactors, proving the superiority of the proposed configuration.

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A kinetic study of the reaction of atomic oxygen with SO2

Cited by 34 publications

References 27 publications

Thermal Dissociation of SO₃ at 1000−1400 K

Thermal Dissociation of SO₃ at 1000−1400 K

Oxidation of Reduced Sulfur Species: Carbon Disulfide

Thermal Integration of Sulfuric Acid and Continuous Catalyst Regeneration of Naphtha Reforming Plants

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A kinetic study of the reaction of atomic oxygen with SO2

Cited by 34 publications

References 27 publications

Thermal Dissociation of SO3 at 1000−1400 K

Thermal Dissociation of SO3 at 1000−1400 K

Oxidation of Reduced Sulfur Species: Carbon Disulfide

Thermal Integration of Sulfuric Acid and Continuous Catalyst Regeneration of Naphtha Reforming Plants

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Thermal Dissociation of SO₃ at 1000−1400 K

Thermal Dissociation of SO₃ at 1000−1400 K