Modeling the sorption dynamics of NaH using a reactive force field.

J.G.O. Ojwang, R.A. Santen, van, G.J. Kramer, A.C.T. Duin, van, W.A. Goddard III

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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 calcd. 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 mol. hydrogen charge transfer during the abstraction process. Results on heat of desorption vs. 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 decompn., we performed a heating run in a mol. dynamics simulation. These runs exhibit a series of drops in potential energy, assocd. with cluster fragmentation and desorption of mol. hydrogen. This is consistent with exptl. evidence that NaH dissocs. at its m.p. into smaller fragments. (c) 2008 American Institute of Physics.
Original languageEnglish
Pages (from-to)164714-1/9
JournalJournal of Chemical Physics
Volume128
Issue number16
DOIs
Publication statusPublished - 2008

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