The role of the multi-body interaction in the de-NOx process on solid catalysts investigated by density functional method

Michiyuki Yamadaya, András Stirling, Hiroaki Himei, Momoji Kubo, Rajappan Vetrivel, Ewa Broclawik, Akira Miyamoto

Research output: Contribution to journalArticlepeer-review

1 Citation (Scopus)


We have performed density functional calculations to investigate the bimolecular CH4 + NOx (x = 1, 2) and the trimolecular NO + CH4 + NO2 reactions which can be assumed to occur in the vicinity of an active site on a de-NOx catalyst. We have shown that the trimolecular reactions can take place very smoothly on a singlet energy hypersurface, while the bimolecular reactions producing unstable radicals are not favorable. We have explained these results with the high energy of the reaction products in the bimolecular reactions and the formation of HNOx molecules yielding negative stabilization energy in the trimolecular reactions with the extra NOx molecules which can be considered as spin traps in these processes. We present the geometrical changes together with the electronic changes occurring in the reactions. The significance of this study is that we could demonstrate that the increased concentration of the reaction partners due to an active site of the catalyst allows reactions which otherwise would be unlikely.

Original languageEnglish
Pages (from-to)189-196
Number of pages8
JournalCatalysis Today
Issue number1-2
Publication statusPublished - 1997 Mar 14


  • Density functional calculation
  • Methane activation
  • NO

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)


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