Mechanisms of Radical Removal by SO2

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Article on mechanisms of radical removal by SO2.

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9 p.

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Rasmussen, Christian Lund; Glarborg, Peter & Marshall, Paul January 1, 2007.

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Article on mechanisms of radical removal by SO2.

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9 p.

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Abstract: It is well established from experiments in premixed, laminar flames, jet-stirred reactors, flow reactors, and batch reactors that SO2 acts to catalyze hydrogen atom removal at stoichiometric and reducing conditions. However, the commonly accepted mechanism for radical removal, SO2 + H(+M) ⇌ HOSO(+M), HOSO + H/OH ⇌ SO2 + H2/H2O, has been challenged by recent theoretical and experimental results. Based on ab initio calculations for key reactions, we update the kinetic model for this chemistry and re-examine the mechanism of fuel/SO2 interactions. We find that the interaction of SO2 with the radical pool is more complex than previously assumed, involving HOSO and SO, as well as, at high temperatures also HSO, SH, and S. The revised mechanism with a high rate constant for H + SO2 recombination and with SO + H2O, rather than SO2 + H2, as major products of the HOSO + H reaction is in agreement with a range of experimental results from batch and flow reactors, as well as laminar flames.

This is the accepted manuscript version of the article. Reprinted with permission from Elsevier Science Ltd., all rights reserved. The final definitive version is available here: http://www.sciencedirect.com/science/article/pii/S154074890600126X

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  • Proceedings of the Combustion Institute, 2007, Amsterdam: Elsevier Science Ltd., pp. 339-347

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  • Publication Title: Proceedings of the Combustion Institute
  • Volume: 31
  • Issue: 1
  • Page Start: 339
  • Page End: 347
  • Peer Reviewed: Yes

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  • January 1, 2007

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  • Oct. 7, 2015, midnight

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Rasmussen, Christian Lund; Glarborg, Peter & Marshall, Paul. Mechanisms of Radical Removal by SO2, article, January 1, 2007; [Amsterdam, Netherlands]. (digital.library.unt.edu/ark:/67531/metadc725872/: accessed July 23, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT College of Arts and Sciences.