Advanced

Development and Application of a ReaxFF Reactive Force Field for Oxidative Dehydrogenation on Vanadium Oxide Catalysts

Chenoweth, Kimberly; van Duin, Adri C. T.; Persson, Petter LU ; Cheng, M.-J.; Oxgaard, J. and Goddard III, W. A. (2008) In Journal of Physical Chemistry C 112(37). p.14645-14654
Abstract
We have developed a new ReaxFF reactive force field to describe accurately reactions of hydrocarbons with vanadium oxide catalysts. The ReaxFF force field parameters have been fit to a large quantum mechanics (QM) training set containing over 700 structures and energetics related to bond dissociations, angle and dihedral distortions, and reactions between hydrocarbons and vanadium oxide clusters. In addition, the training set contains charge distributions for small vanadium oxide clusters and the stabilities of condensed-phase systems. We find that ReaxFF reproduces accurately the QM training set for structures and energetics of small clusters. Most important is that ReaxFF describes accurately the energetics for various oxidation states... (More)
We have developed a new ReaxFF reactive force field to describe accurately reactions of hydrocarbons with vanadium oxide catalysts. The ReaxFF force field parameters have been fit to a large quantum mechanics (QM) training set containing over 700 structures and energetics related to bond dissociations, angle and dihedral distortions, and reactions between hydrocarbons and vanadium oxide clusters. In addition, the training set contains charge distributions for small vanadium oxide clusters and the stabilities of condensed-phase systems. We find that ReaxFF reproduces accurately the QM training set for structures and energetics of small clusters. Most important is that ReaxFF describes accurately the energetics for various oxidation states of the condensed phases, including V2O5, VO2, and V2O3 in addition to metallic V (V0). To demonstrate the capability of the ReaxFF force field for describing catalytic processes involving vanadium oxides, we performed molecular dynamics (MD) simulation for reactions of a gas of methanol exposed to the (001) surface of V2O5. We find that formaldehyde is the major product, in agreement with experiment. These studies find that water desorption from surface VIII sites is facilitated by interlayer bonding. (Less)
Please use this url to cite or link to this publication:
author
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Physical Chemistry C
volume
112
issue
37
pages
14645 - 14654
publisher
The American Chemical Society
external identifiers
  • scopus:53149142090
ISSN
1932-7447
DOI
10.1021/jp802134x
language
English
LU publication?
no
id
f5e3eb06-9adc-4184-a009-9525daf98bc1 (old id 1457456)
date added to LUP
2009-09-01 14:55:17
date last changed
2017-09-17 04:47:24
@article{f5e3eb06-9adc-4184-a009-9525daf98bc1,
  abstract     = {We have developed a new ReaxFF reactive force field to describe accurately reactions of hydrocarbons with vanadium oxide catalysts. The ReaxFF force field parameters have been fit to a large quantum mechanics (QM) training set containing over 700 structures and energetics related to bond dissociations, angle and dihedral distortions, and reactions between hydrocarbons and vanadium oxide clusters. In addition, the training set contains charge distributions for small vanadium oxide clusters and the stabilities of condensed-phase systems. We find that ReaxFF reproduces accurately the QM training set for structures and energetics of small clusters. Most important is that ReaxFF describes accurately the energetics for various oxidation states of the condensed phases, including V2O5, VO2, and V2O3 in addition to metallic V (V0). To demonstrate the capability of the ReaxFF force field for describing catalytic processes involving vanadium oxides, we performed molecular dynamics (MD) simulation for reactions of a gas of methanol exposed to the (001) surface of V2O5. We find that formaldehyde is the major product, in agreement with experiment. These studies find that water desorption from surface VIII sites is facilitated by interlayer bonding.},
  author       = {Chenoweth, Kimberly and van Duin, Adri C. T. and Persson, Petter and Cheng, M.-J. and Oxgaard, J. and Goddard III, W. A.},
  issn         = {1932-7447},
  language     = {eng},
  number       = {37},
  pages        = {14645--14654},
  publisher    = {The American Chemical Society},
  series       = {Journal of Physical Chemistry C},
  title        = {Development and Application of a ReaxFF Reactive Force Field for Oxidative Dehydrogenation on Vanadium Oxide Catalysts},
  url          = {http://dx.doi.org/10.1021/jp802134x},
  volume       = {112},
  year         = {2008},
}