Abstract
Industrial sour gas flaring is difficult to operate appropriately, especially when the gas stream contains high concentrations of sulfur compounds such as hydrogen sulfide and mercaptans. However, most of the detailed combustion mechanisms for hydrocarbons are too complicated, and the computation can be time consuming. In addition, most of the available combustion mechanisms for sulfur compounds are not tailored for sour gas flaring. A reduced combustion mechanism for sour gas will be highly desirable for practical application. In this work, a reduced combustion kinetic mechanism for sour gas combustion, namely the H&S mechanism, was created. This mechanism was validated against experimental data from the literature with proven accuracy. During mechanism analysis, it was found that the addition of H2S had a significant impact on the radical pool. A small amount of H2S leads to a fast buildup of H, OH, and O radicals and a rapid decomposition of CH4. The impact on ignition delay time due to an increase in H2S concentration by 3 vol. % was also analyzed. The impact needs to be compensated by the addition of supplementary fuel. This research will contribute to the clean combustion of sour gas, especially sour gas flares.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Alzueta MU, Bilbao R, Glarborg P (2001) Inhibition and sensitization of fuel oxidation by SO2. Combust Flame 127:2234–2251. https://doi.org/10.1016/S0010-2180(01)00325-X
ANSYS (2016) ANSYS Chemkin-Pro
Binoist M, Labégorre B, Monnet F et al (2003) Kinetic study of the pyrolysis of H2S. Ind Eng Chem Res 42:3943–3951. https://doi.org/10.1021/ie021012r
Boley T, Stuck D, Patel N (2013) Predictive Flare Vent Gas Net Heating Value Through Determination of Average Molecular Weight. In: SAGE Environ. Consult. pp 1–9
Bongartz D, Ghoniem AF (2015) Chemical kinetics mechanism for oxy-fuel combustion of mixtures of hydrogen sulfide and methane. Combust Flame 162:544–553. https://doi.org/10.1016/j.combustflame.2014.08.019
Cerru FG, Kronenburg A, Lindstedt RP (2005) A systematically reduced reaction mechanism for sulphur oxidation. Proc Combust Inst 30:1227–1235. https://doi.org/10.1016/j.proci.2004.08.083
Cerru FG, Kronenburg A, Lindstedt RP (2006) Systematically reduced chemical mechanisms for sulfur oxidation and pyrolysis. Combust Flame 146:437–455. https://doi.org/10.1016/j.combustflame.2006.05.005
Chamberlin DS, Clarke DR (1948) Flame speed of hydrogen sulfide. Proc Symp Combust 1–2:33–35
CHEMKIN Software (2011) Reaction Design CHEMKIN Tutorials Manual. In: CHEMKIN Softw. http://www.ems.psu.edu/~radovic/ChemKin_Tutorial_2-3-7.pdf. Accessed 31 Jan 2021
Chen D, Lou H, Li X, et al (2014) Texas Commission on Environmental Quality (TCEQ) Flare Performance Optimization: DRE/CE vs. Soot Phase I Final Report
Chin HSF, Karant K, Mehrotra AK, Behie LA (2001) The fate of methane in a claus plant reaction furnace. Can J Chem Eng 79:482–490
Chin HSF (2000) The fate of methane in the reaction furnace of a modified claus plant. University of Calgary
Eow JS (2002) Recovery of sulfur from sour acid gas: a review of the technology. Environ Prog 21:143–162. https://doi.org/10.1002/ep.670210312
Fleig D, Alzueta MU, Normann F et al (2013) Measurement and modeling of sulfur trioxide formation in a flow reactor under post-flame conditions. Combust Flame 160:1142–1151. https://doi.org/10.1016/j.combustflame.2013.02.002
Frenklach M, Lee JH, White JN, Gardiner WC (1981) Oxidation of hydrogen sulfide. Combust Flame 41:1–16. https://doi.org/10.1016/0010-2180(81)90035-3
Giménez-López J, Martínez M, Millera A et al (2011) SO2 effects on CO oxidation in a CO2 atmosphere, characteristic of oxy-fuel conditions. Combust Flame 158:48–56. https://doi.org/10.1016/j.combustflame.2010.07.017
Glarborg P, Bentzen LLB (2008) Chemical effects of a high CO2 concentration in oxy-fuel combustion of methane. Energy Fuels 22:291–296. https://doi.org/10.1021/ef7005854
Glarborg P, Kubel D, Dam-Johansen K et al (1996) Impact of SO2 and NO on CO oxidation under post-flame conditions. Int J Chem Kinet 28:773–790. https://doi.org/10.1002/(SICI)1097-4601(1996)28:10%3c773::AID-KIN8%3e3.0.CO;2-K
Hughes KJ, Turányi T, Clague AR, Pilling MJ (2001) Development and testing of a comprehensive chemical mechanism for the oxidation of methane. Int J Chem Kinet 33:513–538. https://doi.org/10.1002/kin.1048
Kéromnès A, Metcalfe WK, Heufer KA et al (2013) An experimental and detailed chemical kinetic modeling study of hydrogen and syngas mixture oxidation at elevated pressures. Combust Flame 160:995–1011. https://doi.org/10.1016/J.COMBUSTFLAME.2013.01.001
Levy A, Merryman EL (1965) The microstructure of hydrogen sulphide flames. Combust Flame 9:229–240. https://doi.org/10.1016/0010-2180(65)90089-1
Levy A, Merryman EL, Reid WT (1970) Mechanisms of Formation of Sulfur Oxides in Combustion. Environ Sci Technol 4:653–662. https://doi.org/10.1021/es60043a005
Marinov NM, Pitz WJ, Westbrook CK, Castaldi MJ, Senkan SM (1996) Modeling of aromatic and polycyclic aromatic hydrocarbon formation in premixed methane and ethane flames. Comb Sci Technol 116(1–6):211–287
Mathieu O, Deguillaume F, Petersen EL (2014) Effects of H2S addition on hydrogen ignition behind reflected shock waves: experiments and modeling. Combust Flame 161:23–36. https://doi.org/10.1016/J.COMBUSTFLAME.2013.07.011
Merryman EL, Levy A (1967) Kinetics of sulfur-oxide formation in flames: II. low pressure H2S flames. J Air Pollut Control Assoc 17:800–806. https://doi.org/10.1080/00022470.1967.10469073
Merryman EL, Levy A (1972) Disulfur and the lower oxides of sulfur in hydrogen sulfide flames. J Phys Chem 76:1925–1931. https://doi.org/10.1021/j100658a002
Metcalfe WK, Burke SM, Ahmed SS, Curran HJ (2013) A hierarchical and comparative kinetic modeling study of C1–C2 hydrocarbon and oxygenated fuels. Int J Chem Kinet 45:638–675. https://doi.org/10.1002/kin.20802
Mohammed S, Raj A, Al Shoaibi A, Sivashanmugam P (2015) Formation of polycyclic aromatic hydrocarbons in Claus process from contaminants in H2S feed gas. Chem Eng Sci 137:91–105. https://doi.org/10.1016/j.ces.2015.06.029
Petherbridge JR, May PW, Shallcross DE et al (2003) Simulation of H-C-S containing gas mixtures relevant to diamond chemical vapour deposition. Diam Relat Mater 12:2178–2185. https://doi.org/10.1016/S0925-9635(03)00294-2
Selim H, Gupta AK, Sassi M (2009) Reduced mechanism for the oxidation of hydrogen sulfide. In: 47th AIAA Aerospace Sciences Meeting. Orlando, FL, USA, pp 263–278
Sendt K, Jazbec M, Haynes BS (2002) Chemical kinetic modeling of the H/S system: H2S thermolysis and H2 sulfidation. Proc Combust Inst 29:2439–2446. https://doi.org/10.1016/s1540-7489(02)80297-8
TCEQ (2010) TCEQ 2010 Flare Study Final Report
Tsuchiya K, Kamiya K, Matsui H (1997) Studies on the oxidation mechanism of H2S based on direct examination of the key reactions. Int J Chem Kinet 29:57–66. https://doi.org/10.1002/(SICI)1097-4601(1997)29:1%3c57::AID-KIN7%3e3.0.CO;2-K
US EPA (1992) 40 CFR § 63.671 - Requirements for flare monitoring systems. In: Leg. Inf. Inst. https://www.law.cornell.edu/cfr/text/40/63.671. Accessed 27 Aug 2019
US EPA (2012) Parameters for properly designed and operated flares
Wang A, Lou HH, Chen D et al (2016) Combustion mechanism development and CFD simulation for the prediction of soot emission during flaring. Front Chem Sci Eng 10:459–471. https://doi.org/10.1007/s11705-016-1594-y
Wang H, You X, Joshi A V, et al (2007) USC Mech Version II. High-Temperature Combustion Reaction Model of H2/CO/C1-C4 Compounds. University of Southern California
Wendt JOL, Ekmann JM (1975) Effect of fuel sulfur species on nitrogen oxide emissions from premixed flames. Combust Flame 25:355–360. https://doi.org/10.1016/0010-2180(75)90107-8
Yossefi D, Ashcroft SJ, Hacohen J et al (1995) Combustion of methane and ethane with CO2 replacing N2 as a diluent. Modelling of combined effects of detailed chemical kinetics and thermal properties on the early stages of combustion. Fuel 74:1061–1071. https://doi.org/10.1016/0016-2361(95)00048-A
Zhou C, Sendt K, Haynes BS (2013) Experimental and kinetic modelling study of H2S oxidation. Proc Combust Inst 34:625–632. https://doi.org/10.1016/j.proci.2012.05.083
Acknowledgements
The authors wish to thank all who assisted in conducting this work.
Funding
This research was supported by Lamar University Center for Midstream Management and Science (CMMS) and Lamar University College of Engineering.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declared that there is no conflict of interest.
Additional information
Editorial responsibility: Maryam Shabani.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Gai, H., Jayswal, A., Fang, J. et al. Development of a reduced mechanism for sour gas flaring. Int. J. Environ. Sci. Technol. 19, 8195–8206 (2022). https://doi.org/10.1007/s13762-021-03699-z
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13762-021-03699-z