skip to main content

Density Functional Theory Study of Nitrous Oxide Decomposition over Fe- and Co-ZSM-5

Ryder, Jason A ; Chakraborty, Arup K ; Bell, Alexis T

The journal of physical chemistry. B, 2002-07-18, Vol.106 (28), p.7059-7064 [Peer Reviewed Journal]

Full text available

Citations Cited by
  • Title:
    Density Functional Theory Study of Nitrous Oxide Decomposition over Fe- and Co-ZSM-5
  • Author: Ryder, Jason A ; Chakraborty, Arup K ; Bell, Alexis T
  • Subjects: Density functionals ; Iron alloys ; Nitrous oxide ; Research
  • Is Part Of: The journal of physical chemistry. B, 2002-07-18, Vol.106 (28), p.7059-7064
  • Description: Iron- and cobalt-exchanged ZSM-5 are active catalysts for the dissociation of nitrous oxide. In this study, density functional theory was used to assess a possible reaction pathway for the catalytic dissociation of N2O. The active center was taken to be mononuclear [FeO]+ or [CoO]+, and the surrounding portion of the zeolite was represented by a 24-atom cluster. The first step of N2O decomposition involves the formation of [FeO2]+ or [CoO2]+ and the release of N2. The metal-oxo species produced in this step then reacts with N2O again, to release N2 and O2. The apparent activation energies for N2O dissociation in Fe−ZSM-5 and Co−ZSM-5 are 39.4 and 34.6 kcal/mol, respectively. The preexponential factor for the apparent first-order rate coefficient is estimated to be of the order 107 s-1 Pa -. Although the calculated activation energy for Fe−ZSM-5 is in good agreement with that measured experimentally, the value of the preexponential factor is an order of magnitude smaller than that observed. The calculated activation energy for Co−ZSM-5 is higher than that reported experimentally. However, consistent with experiment, the rate of N2O decomposition on Co−ZSM-5 is predicted to be significantly higher than that on Fe−ZSM-5.
  • Publisher: American Chemical Society
  • Language: English
  • Identifier: ISSN: 1520-6106
    EISSN: 1520-5207
    DOI: 10.1021/jp014705e

Searching Remote Databases, Please Wait