Experimental and kinetic modelling study of H2S oxidation

Zhou, Chenlai; Sendt, Karina; Haynes, Brian S.

doi:10.1016/j.proci.2012.05.083

Cited by 91 publications

(102 citation statements)

References 24 publications

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“…Recently, Zhou et al [35] presented a mechanism for H 2 S oxidation that puts more emphasis on the chemistry of disulfur species. Since these were found to be particularly important near stoichiometric conditions, this mechanism was chosen as the basic sulfur mechanism.…”

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

“…The thermodynamic data was taken from AramcoMech 1.3 and Zhou et al [35], except for the enthalpy of formation of the mercapto radical (SH), which was set to ∆H 0 f,298 (SH) = 33.8 kcal/mol. This is in agreement with the recent recommendations of Goos et al [36] and Denis [37] while improving overall agreement with the experimental data used for validation.…”

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

“…• the laminar burning velocity of H 2 S in air at atmospheric pressure [39][40][41][42] • the ignition delay time of H 2 S in air as measured by Frenklach et al [29] • the pyrolysis of H 2 S in the experiment of Hawboldt et al [43] • the H 2 S flow reactor experiment of Zhou et al [35] The exact points used, the corresponding target values, and the assigned weights are listed in Table 1. For the laminar burning velocity (target 1), a target range was chosen to account for the scatter of the data points from the different experiments.…”

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

“…For the ignition delay time (targets 2-5), target ranges were chosen because the selection of a single data point led to arbitrarily different results. For the flow reactor experiment of Zhou et al [35], we only considered the cases with an equivalence ratio of Φ = 0.8 (targets 8-12) because they are closer to the conditions around stoichiometry that occur in oxy-fuel combustion than the third case presented therein (Φ = 0.15).…”

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

“…In the following, they are referred to as 'Optimization 1-12', 'Optimization 1-7', and 'Optimization 8-12', where the numbers are the target numbers given in Table 1. These combinations correspond to an optimization with respect to all experiments mentioned above, all experiments except the H 2 S flow reactor of Zhou et al [35], and only the H 2 S flow reactor, respectively. The decision variables used in the optimization were the pre-exponential factors for the rate constants of 15 reactions in the sulfur mechanism to which the results for the target cases were particularly sensitive.…”

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

See 4 more Smart Citations

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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Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

Section: Mechanism Selection and Optimizationmentioning

confidence: 99%

See 3 more Smart Citations

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

Bongartz

Ghoniem

2015

Combustion and Flame

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A detailed reaction mechanism for elemental sulphur combustion in the furnace of sulphuric acid plants

2021

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Elemental sulphur combustion is traditionally used to generate SO2 to produce sulphuric acid that is consumed in chemical industries, but is now also being considered as an energy vector for power generation. Despite the fact that sulphur combustion has been practiced for decades, there are limited reaction mechanisms for its combustion chemistry, which is critical for the optimization of the sulphuric acid production process to maximize efficiency and reduce cost. In this paper, a detailed reaction mechanism is developed and validated with different sets of experimental data from lab‐scale and industrial plant studies. The reaction mechanism is used to conduct sulphur furnace simulations, where the effects of feed air/sulphur ratio and oxygen enrichment of air stream on furnace temperature and the concentrations of SO2, SO3, and O2 are investigated. The dominant reaction pathways in sulphur combustion, particularly for the production of SO2 and SO3, are identified. It was found that the feed air/sulphur ratio monitors the furnace temperature and can be used to obtain the desired O2/SO2 ratio at the furnace exit for the optimal operation of catalytic converter (for SO2 oxidation to SO3) that follows the furnace in the sulphuric acid plant. Moreover, high oxygen enrichment above 35% (while maintaining the desired O2/SO2 ratio at the furnace exit) significantly increased the furnace capacity through reduced total gas flow (thus decreasing blower energy requirement and equipment size). The developed reaction mechanism provides a method to obtain optimized furnace parameters to achieve high efficiency and reduced costs in sulphuric acid plants.

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An ab initio‐based global potential energy surface for the SH₃ system and full‐dimensional state‐to‐state quantum dynamics study for the H₂ + HS → H₂S + H reaction

Chen

Liu

et al. 2018

J Comput Chem

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An accurate potential energy surface for the ground electronic state of SH 3 system has been constructed with 41,882 high level ab initio energy points and the neural network fitting method. The time-dependent wave packet method has been used to calculate the first state-to-state differential cross sections for the title reaction up to 1.2 eV in full dimensions, based on the reactant-product decoupling scheme. It is found that the majority of H 2 S are produced in the ground vibrational state, with a large fraction of available energy for the reaction ending up as product translational motion. The differential cross sections at the threshold energy are dominated by a very narrow peak in the backward direction. With the increase of collision energy, the width of the angular distribution increases considerably, which is a typical feature of a direct reaction via abstract mechanism, similar to the H 2 + OH ! H 2 O + H reaction.

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Experimental and kinetic modelling study of H2S oxidation

Cited by 91 publications

References 24 publications

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

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

A detailed reaction mechanism for elemental sulphur combustion in the furnace of sulphuric acid plants

An ab initio‐based global potential energy surface for the SH₃ system and full‐dimensional state‐to‐state quantum dynamics study for the H₂ + HS → H₂S + H reaction

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Experimental and kinetic modelling study of H2S oxidation

Cited by 91 publications

References 24 publications

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

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

A detailed reaction mechanism for elemental sulphur combustion in the furnace of sulphuric acid plants

An ab initio‐based global potential energy surface for the SH3 system and full‐dimensional state‐to‐state quantum dynamics study for the H2 + HS → H2S + H reaction

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An ab initio‐based global potential energy surface for the SH₃ system and full‐dimensional state‐to‐state quantum dynamics study for the H₂ + HS → H₂S + H reaction