Temperature Dependence of the Oxidation of Hydrogen with Sulfur Dioxide

Capa

Citar

Texto integral

Acesso aberto Acesso aberto
Acesso é fechado Acesso está concedido
Acesso é fechado Somente assinantes

Resumo

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.

Sobre autores

P. Gukasyan

Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia

Email: petros@ichph.sci.am
Yerevan, Armenia

E. Makaryan

Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia

Email: makaryan@mail.ru
Yerevan, Armenia

A. Arutyunyan

Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia

Email: makaryan@mail.ru
Yerevan, Armenia

A. Davtyan

Nalbandyan Institute of Chemical Physics, National Academy of Sciences of Armenia

Autor responsável pela correspondência
Email: makaryan@mail.ru
Yerevan, Armenia

Bibliografia

  1. Справочник компании // Норникель 2017 г.
  2. Елисеев А.В. // Изв. РAH. Физикa aтмocфepы и oкeaнa. 2015. Т. 51. № 6. С. 673.
  3. Елисеев А.В., Чжан М., Гизатуллин Р.Д., Алтухова А.В. // Изв. РAH. Физикa aтмocфepы и oкeaнa. 2019. Т. 55. № 1. С. 41.
  4. Хайрулин С.Р., Керженцев М.А., Яшкин С.А. и др. // Химия в интересах устойчивого развития. 2015. Т. 23. С. 469.
  5. Rasmusen G.L., Glarborg P., Marshal P. // Proc. Combustion Inst. 2007. V. 31. P. 339.
  6. Гукасян П.С. // Хим. журн. Армении. 2009. Т. 61. № 3–4. С. 303.
  7. Mantashyan A.A., Wang H., Avetisyan A.M., Makaryan E.M. // Хим. журн. Армении. 2006. V. 59. № 4. P. 35.
  8. Mantashyan A.A. // Rus. J. of Physical Chemistry A. 2021. V. 15. № 1. P. 233.
  9. Манташян А.А., Макарян Э.М., Аракелян Л.С. // Физика горения и взрыва. 2019. Т. 55. № 2. С. 3.
  10. Гукасян П.С., Макарян Э., Давтян А., Арутюнян А. // Хим. журн. Армении. 2022. Т. 75. № 1. С. 3.
  11. Han G.B., Park N.-K., Lee T.J. // Ind. Eng. Chem. Res. 2009. V. 48. № 23. P. 10307.
  12. Ishiguro A., Lio X., Nakajima T. // J. Catal. 2002. V. 206. № 1. P. 159.
  13. Zhu T., Draher A., Flytzani-Stephanopoulos M. // Appl. Catal. B: Environ. 1999. V. 21. P. 103.
  14. Han G.B., Park N.-K., Yoon S.H., Lee T.J. // Ind. Eng. Chem. Res. 2008. V. 47. № 14. P. 4658.
  15. Weigang Wang, Mingyuan Liu, Tiantian Wang & andere // Nature Communications. 2021. V. 10. P. 1.
  16. 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.
  17. Blitz M.A., Hughes K.J., Pilling M.J., Robertson S.H. // J. Phys. Chem. A. 2006. V. 110. P. 2996.
  18. Stickel R.E., Chin M., Daykin E.P. et al. // J. Phys. Chem. 1993. V. 97. P. 13653.
  19. Baulch D.L., Drysdale D.D., Horne D.G. // Symp. Int. Combust. Proc. 1973. V. 14. P. 107.
  20. Schofield K. // J. Phys. Chem. Ref. Data.1973. V. 2. P. 25.
  21. Sutherland J.W., Michael J.V., Pirraglia A.N. et al. // Symp. Int. Combust. Proc. 1988. Issue 1. V. 21. P. 929.
  22. Becke A.D. // J. Chem. Phys. 1993. V. 98. P. 5648.
  23. Montgomery J.A., Frisch M.J., Ochterski J.W., & Petersson G. A. // Ibid. 2000.V. 112 (15). P. 6532.
  24. 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
  25. Frisch M.J., Trucks G.W., Schlegel H.B. et al. Gaussian 16, Revision C.01.Gaussian Inc. Wallingford CT, 2016.
  26. Dennington R., Keith T.A., Millam J.M. Gauss View Version 6. Semichem Inc., Shawnee Mission, KS. 2016.

Arquivos suplementares

Arquivos suplementares
Ação
1. JATS XML
Baixar
2.

Baixar (167KB)
Metadados
3.

Baixar (34KB)
Metadados
4.

Baixar (49KB)
Metadados
5.

Baixar (124KB)
Metadados
6.

Baixar (36KB)
Metadados
7.

Baixar (183KB)
Metadados

Declaração de direitos autorais © П.С. Гукасян, Э.М. Макарян, А.А. Арутюнян, А.Г. Давтян, 2023