Temperature Dependence of the Oxidation of Hydrogen with Sulfur Dioxide

P. S. Gukasyan; Гукасян П. С.; E. M. Makaryan; Макарян Э. М.; A. A. Arutyunyan; Арутюнян А. А.; A. G. Davtyan; Давтян А. Г.

doi:10.31857/S0044453723080083

Temperature Dependence of the Oxidation of Hydrogen with Sulfur Dioxide

Authors: Gukasyan P.S.¹, Makaryan E.M.¹, Arutyunyan A.A.¹, Davtyan A.G.¹
Affiliations:
1. Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia
Issue: Vol 97, No 8 (2023)
Pages: 1200-1206
Section: ФИЗИЧЕСКАЯ ХИМИЯ ПРОЦЕССОВ ГОРЕНИЯ И ВЗРЫВА
Submitted: 15.10.2023
Published: 01.08.2023
URL: https://bakhtiniada.ru/0044-4537/article/view/136676
DOI: https://doi.org/10.31857/S0044453723080083
EDN: https://elibrary.ru/QUVYUB
ID: 136676

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Abstract
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Abstract

An experimental study is performed of the mechanism of sulfur dioxide–hydrogen interaction (4Н2 + 2SО2 → S2 + 4H2О) at temperatures of 623, 673, 723, and 773 K and a pressure of 198 Torr. The mechanism is analyzed via mathematical modeling. It is found to be a chain reaction of hydrogen oxidation with sulfur dioxide, which results in the formation of molecular sulfur (S2). The process is characterized by negative Gibbs free energy ΔG723 = −49.950 kcal/mol. The potential energy surface of the (HOSO + HOSO) system is studied by various means of quantum chemistry, and the thermodynamic parameters of the НОSO + НОSO → SO + SO2 + Н2О reaction are determined. A new mechanism of the reaction, supplemented by elementary acts, is discussed. Good agreement is found between energies of activation determined experimentally and calculated using data from our numerical kinetic analysis.

Keywords

sulfur, sulfur dioxide, chain reaction, kinetic analysis

References

Справочник компании // Норникель 2017 г.
Елисеев А.В. // Изв. РAH. Физикa aтмocфepы и oкeaнa. 2015. Т. 51. № 6. С. 673.
Елисеев А.В., Чжан М., Гизатуллин Р.Д., Алтухова А.В. // Изв. РAH. Физикa aтмocфepы и oкeaнa. 2019. Т. 55. № 1. С. 41.
Хайрулин С.Р., Керженцев М.А., Яшкин С.А. и др. // Химия в интересах устойчивого развития. 2015. Т. 23. С. 469.
Rasmusen G.L., Glarborg P., Marshal P. // Proc. Combustion Inst. 2007. V. 31. P. 339.
Гукасян П.С. // Хим. журн. Армении. 2009. Т. 61. № 3–4. С. 303.
Mantashyan A.A., Wang H., Avetisyan A.M., Makaryan E.M. // Хим. журн. Армении. 2006. V. 59. № 4. P. 35.
Mantashyan A.A. // Rus. J. of Physical Chemistry A. 2021. V. 15. № 1. P. 233.
Манташян А.А., Макарян Э.М., Аракелян Л.С. // Физика горения и взрыва. 2019. Т. 55. № 2. С. 3.
Гукасян П.С., Макарян Э., Давтян А., Арутюнян А. // Хим. журн. Армении. 2022. Т. 75. № 1. С. 3.
Han G.B., Park N.-K., Lee T.J. // Ind. Eng. Chem. Res. 2009. V. 48. № 23. P. 10307.
Ishiguro A., Lio X., Nakajima T. // J. Catal. 2002. V. 206. № 1. P. 159.
Zhu T., Draher A., Flytzani-Stephanopoulos M. // Appl. Catal. B: Environ. 1999. V. 21. P. 103.
Han G.B., Park N.-K., Yoon S.H., Lee T.J. // Ind. Eng. Chem. Res. 2008. V. 47. № 14. P. 4658.
Weigang Wang, Mingyuan Liu, Tiantian Wang & andere // Nature Communications. 2021. V. 10. P. 1.
Lutz A.E., Kee R.J., Miller J.A. SENKIN: A FORTRAN-Program for Predicting Homogeneous Gas Phase Chemical Kinetics with Sensitivity Analysis // Sandia Nat. Lab. Rep. SAND-87-8248. Livermore, CA, 1987. Available at: http: www.osti.gov/scitech/biblio/5371815.
Blitz M.A., Hughes K.J., Pilling M.J., Robertson S.H. // J. Phys. Chem. A. 2006. V. 110. P. 2996.
Stickel R.E., Chin M., Daykin E.P. et al. // J. Phys. Chem. 1993. V. 97. P. 13653.
Baulch D.L., Drysdale D.D., Horne D.G. // Symp. Int. Combust. Proc. 1973. V. 14. P. 107.
Schofield K. // J. Phys. Chem. Ref. Data.1973. V. 2. P. 25.
Sutherland J.W., Michael J.V., Pirraglia A.N. et al. // Symp. Int. Combust. Proc. 1988. Issue 1. V. 21. P. 929.
Becke A.D. // J. Chem. Phys. 1993. V. 98. P. 5648.
Montgomery J.A., Frisch M.J., Ochterski J.W., & Petersson G. A. // Ibid. 2000.V. 112 (15). P. 6532.
Frisch M.J., Head-Gordon M., and Pople J.A. // Chem. Phys. Lett. 1990. V. 166. P. 275. https://doi.org/10.1016/0009-2614(90)80029-D
Frisch M.J., Trucks G.W., Schlegel H.B. et al. Gaussian 16, Revision C.01.Gaussian Inc. Wallingford CT, 2016.
Dennington R., Keith T.A., Millam J.M. Gauss View Version 6. Semichem Inc., Shawnee Mission, KS. 2016.