The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study

Farjamnia, Azar; Jackson, Bret

doi:10.1063/1.4976132

The dissociative chemisorption of CO ₂ on Ni(100): A quantum dynamics study

Journal Article · Tue Feb 21 00:00:00 EST 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4976132· OSTI ID:1344088

Farjamnia, Azar ^[1]; ^[2]

Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry; University of Massachuetts, Amherst
Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry

A quantum approach based on an expansion in vibrationally adiabatic eigenstates is used to explore the dissociative chemisorption of CO₂ on Ni(100). The largest barrier to reaction corresponds to the formation of a bent anionic molecular precursor, bound to the surface by about 0.24 eV. The barrier to dissociation from this state is small. In our computed dissociative sticking probabilities on Ni(100) for molecules, the ground states are in very good agreement with available experimental data, reasonably reproducing the variation in reactivity with collision energy. Vibrational excitation of the incident CO₂ can enhance reactivity, particularly for incident energies at or below threshold, and there is clear mode specific behavior. Both the vibrational enhancement and the increase in dissociative sticking with surface temperature are much weaker than that found in recent studies of methane and water dissociative chemisorption. The energetics for CO₂ adsorption and dissociation on the stepped Ni(711) surface are found to be similar to that on Ni(100), except that the barrier to dissociation from the anionic precursor is even smaller on Ni(711). Here, we predict that the dissociative sticking behavior is similar on the two surfaces.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Massachusetts, Amherst, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: FG02-87ER13744

OSTI ID:: 1344088

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 7 Vol. 146; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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