Modeling the sorption dynamics of NaH using a reactive force field

J. G.O. Ojwang, Rutger Van Santen, Gert Jan Kramer, Adri C.T. Van Duin, William A. Goddard

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

We have parametrized a reactive force field for NaH, ReaxFFNaH, against a training set of ab initio derived data. To ascertain that ReaxFFNaH is properly parametrized, a comparison between ab initio heats of formation of small representative NaH clusters with ReaxFFNaH was done. The results and trend of ReaxFFNaH are found to be consistent with ab initio values. Further validation includes comparing the equations of state of condensed phases of Na and NaH as calculated from ab initio and ReaxFFNaH. There is a good match between the two results, showing that ReaxFFNaH is correctly parametrized by the ab initio training set. ReaxFFNaH has been used to study the dynamics of hydrogen desorption in NaH particles. We find that ReaxFFNaH properly describes the surface molecular hydrogen charge transfer during the abstraction process. Results on heat of desorption versus cluster size shows that there is a strong dependence on the heat of desorption on the particle size, which implies that nanostructuring enhances desorption process. To gain more insight into the structural transformations of NaH during thermal decomposition, we performed a heating run in a molecular dynamics simulation. These runs exhibit a series of drops in potential energy, associated with cluster fragmentation and desorption of molecular hydrogen. This is consistent with experimental evidence that NaH dissociates at its melting point into smaller fragments.

Original languageEnglish (US)
Article number164714
JournalJournal of Chemical Physics
Volume128
Issue number16
DOIs
StatePublished - May 8 2008

Fingerprint

sorption
field theory (physics)
Sorption
Desorption
desorption
Hydrogen
education
hydrogen
heat
heat of formation
Potential energy
Equations of state
thermal decomposition
melting points
Melting point
Molecular dynamics
Charge transfer
fragmentation
Pyrolysis
equations of state

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Ojwang, J. G.O. ; Van Santen, Rutger ; Kramer, Gert Jan ; Van Duin, Adri C.T. ; Goddard, William A. / Modeling the sorption dynamics of NaH using a reactive force field. In: Journal of Chemical Physics. 2008 ; Vol. 128, No. 16.
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Modeling the sorption dynamics of NaH using a reactive force field. / Ojwang, J. G.O.; Van Santen, Rutger; Kramer, Gert Jan; Van Duin, Adri C.T.; Goddard, William A.

In: Journal of Chemical Physics, Vol. 128, No. 16, 164714, 08.05.2008.

Research output: Contribution to journalArticle

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