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Published September 18, 2008 | Supplemental Material
Journal Article Open

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

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 V_2O_5, VO_2, and V_2O_3 in addition to metallic V(V^0). 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 V_2O_5. 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.

Additional Information

© 2008 American Chemical Society. Received 11 March 2008. Published online 25 July 2008. Published in print 18 September 2008. This research was supported, in part, by funds from NSF (ITR-DMR-0427177) and ONR (N00014-05-1-0778). Note Added After ASAP Publication: This article was posted ASAP on July 25, 2008 in The Journal of Physical Chemistry A. After ASAP, the paper was reassigned to The Journal of Physical Chemistry C. The corrected version was posted on August 19, 2008.

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Created:
August 19, 2023
Modified:
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