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Development of the ReaxFF Reactive Force Field for Mechanistic Studies of Catalytic Selective Oxidation Processes on BiMoOx

Goddard III, W. A. ; van Duin, A. C. T. ; Chenoweth, K. ; Cheng, M.-J. ; Pudar, S. ; Oxgaard, J. ; Merinov, B. ; Yang, Y. H. and Persson, Petter LU (2006) In Topics in Catalysis 38(1-3). p.93-103
Abstract
We have developed a new reactive force field, ReaxFF, for use in molecular dynamics (MD) simulations to investigate the structures and reactive dynamics of complex metal oxide catalysts. The parameters in ReaxFF are derived directly from QM and have been validated to provide reasonable accuracy for a wide variety of reactions. We report the use of ReaxFF to study the activation and conversion of propene to acrolein by various metal oxide surfaces. Using high-remperature MD-simulations on metal oxides slabs exposed to a propene gas phase we find that (1) Propene is not activated by MoO3 but it is activated by amorphous Bi2O3 to form allyl which does not get oxidized by the surface; (2) Propene is activated by Bi2Mo3O12 to form an... (More)
We have developed a new reactive force field, ReaxFF, for use in molecular dynamics (MD) simulations to investigate the structures and reactive dynamics of complex metal oxide catalysts. The parameters in ReaxFF are derived directly from QM and have been validated to provide reasonable accuracy for a wide variety of reactions. We report the use of ReaxFF to study the activation and conversion of propene to acrolein by various metal oxide surfaces. Using high-remperature MD-simulations on metal oxides slabs exposed to a propene gas phase we find that (1) Propene is not activated by MoO3 but it is activated by amorphous Bi2O3 to form allyl which does not get oxidized by the surface; (2) Propene is activated by Bi2Mo3O12 to form an allyl-radical and the hydrogen gets abstracted by a Mo=O bond, which is bridged via an O to a Bi-site; (3) Propene is activated over V2O5 to form an allyl, which is then selectively oxidized on the surface to form acrolein. The propene reations on V2O5 occur at lower temperatures than on Bi2O3 or Bi2Mo3O12. The results are all consistent with experimental observations, encouraging us that such investigations will enhance our mechanistic understanding of catalytic hydrocarbon oxidation sufficiently to suggest modifications for improving efficiency and/or selectivity. (Less)
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author
; ; ; ; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
subject
in
Topics in Catalysis
volume
38
issue
1-3
pages
93 - 103
publisher
Springer
external identifiers
  • scopus:33749150817
ISSN
1572-9028
DOI
10.1007/s11244-006-0074-x
language
English
LU publication?
no
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
id
c13011d7-64bb-4633-aacd-ad76490b46d7 (old id 1457602)
date added to LUP
2016-04-01 16:18:01
date last changed
2022-03-07 05:00:38
@article{c13011d7-64bb-4633-aacd-ad76490b46d7,
  abstract     = {{We have developed a new reactive force field, ReaxFF, for use in molecular dynamics (MD) simulations to investigate the structures and reactive dynamics of complex metal oxide catalysts. The parameters in ReaxFF are derived directly from QM and have been validated to provide reasonable accuracy for a wide variety of reactions. We report the use of ReaxFF to study the activation and conversion of propene to acrolein by various metal oxide surfaces. Using high-remperature MD-simulations on metal oxides slabs exposed to a propene gas phase we find that (1) Propene is not activated by MoO3 but it is activated by amorphous Bi2O3 to form allyl which does not get oxidized by the surface; (2) Propene is activated by Bi2Mo3O12 to form an allyl-radical and the hydrogen gets abstracted by a Mo=O bond, which is bridged via an O to a Bi-site; (3) Propene is activated over V2O5 to form an allyl, which is then selectively oxidized on the surface to form acrolein. The propene reations on V2O5 occur at lower temperatures than on Bi2O3 or Bi2Mo3O12. The results are all consistent with experimental observations, encouraging us that such investigations will enhance our mechanistic understanding of catalytic hydrocarbon oxidation sufficiently to suggest modifications for improving efficiency and/or selectivity.}},
  author       = {{Goddard III, W. A. and van Duin, A. C. T. and Chenoweth, K. and Cheng, M.-J. and Pudar, S. and Oxgaard, J. and Merinov, B. and Yang, Y. H. and Persson, Petter}},
  issn         = {{1572-9028}},
  language     = {{eng}},
  number       = {{1-3}},
  pages        = {{93--103}},
  publisher    = {{Springer}},
  series       = {{Topics in Catalysis}},
  title        = {{Development of the ReaxFF Reactive Force Field for Mechanistic Studies of Catalytic Selective Oxidation Processes on BiMoOx}},
  url          = {{http://dx.doi.org/10.1007/s11244-006-0074-x}},
  doi          = {{10.1007/s11244-006-0074-x}},
  volume       = {{38}},
  year         = {{2006}},
}