Development and application of a ReaxFF reactive force field for oxidative dehydrogenation on vanadium oxide catalysts

Kimberly Chenoweth, Adri C.T. Van Duin, Petter Persson, Mu-Jeng Cheng, Jonas Oxgaard, William A. Goddard

Research output: Contribution to journalArticle

85 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)14645-14654
Number of pages10
JournalJournal of Physical Chemistry C
Volume112
Issue number37
DOIs
Publication statusPublished - 2008 Sep 18

Fingerprint

Vanadium
vanadium oxides
Dehydrogenation
dehydrogenation
Oxides
field theory (physics)
catalysts
Catalysts
education
Quantum theory
Hydrocarbons
quantum mechanics
hydrocarbons
Charge distribution
formaldehyde
Formaldehyde
charge distribution
Methanol
Molecular dynamics
interlayers

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Chenoweth, Kimberly ; Van Duin, Adri C.T. ; Persson, Petter ; Cheng, Mu-Jeng ; Oxgaard, Jonas ; Goddard, William A. / Development and application of a ReaxFF reactive force field for oxidative dehydrogenation on vanadium oxide catalysts. In: Journal of Physical Chemistry C. 2008 ; Vol. 112, No. 37. pp. 14645-14654.
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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; Cheng, Mu-Jeng; Oxgaard, Jonas; Goddard, William A.

In: Journal of Physical Chemistry C, Vol. 112, No. 37, 18.09.2008, p. 14645-14654.

Research output: Contribution to journalArticle

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