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Title: Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity

Abstract

We performed a comparative study of mode-selectivity of water dissociation on Ni(100), Ni(110), and Ni(111) surfaces at the same level of theory using a fully quantum approach based on the reaction path Hamiltonian. Calculations show that the barrier to water dissociation on the Ni(110) surface is significantly lower compared to its close-packed counterparts. Transition states for this reaction on all three surfaces involve the elongation of one of the O–H bonds. Furthermore, a significant decrease in the symmetric stretching and bending mode frequencies near the transition state is observed in all three cases and in the vibrational adiabatic approximation, excitation of these softened modes results in a significant enhancement in reactivity. Inclusion of non-adiabatic couplings between modes results in the asymmetric stretching mode showing a similar enhancement of reactivity as the symmetric stretching mode. Dissociation probabilities calculated at a surface temperature of 300 K showed higher reactivity at lower collision energies compared to that of the static surface case, underlining the importance of lattice motion in enhancing reactivity. Mode selective behavior is similar on all the surfaces. Molecules with one-quantum of vibrational excitation in the symmetric stretch, at lower energies (up to 0.45 eV), are more reactive on Ni(110) thanmore » the Ni(100) and Ni(111) surfaces. But, the dissociation probabilities approach saturation on all the surfaces at higher incident energy values. Ultimately, Ni(110) is found to be highly reactive toward water dissociation among the low-index nickel surfaces owing to a low reaction barrier resulting from the openness and corrugation of the surface. These results show that the mode-selective behavior does not vary with different crystal facets of Ni qualitatively, but there is a significant quantitative effect.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Indian Inst. of Science Education and Resesarch Kolkata, Mohanpur (India)
  2. Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Massachusetts, Amherst, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1344098
Alternate Identifier(s):
OSTI ID: 1361779
Grant/Contract Number:  
FG02-87ER13744
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 7; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Seenivasan, H., Jackson, Bret, and Tiwari, Ashwani K. Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity. United States: N. p., 2017. Web. doi:10.1063/1.4976133.
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Seenivasan, H., Jackson, Bret, & Tiwari, Ashwani K. Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity. United States. https://doi.org/10.1063/1.4976133
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Seenivasan, H., Jackson, Bret, and Tiwari, Ashwani K. Fri . "Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity". United States. https://doi.org/10.1063/1.4976133. https://www.osti.gov/servlets/purl/1344098.
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@article{osti_1344098,
title = {Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity},
author = {Seenivasan, H. and Jackson, Bret and Tiwari, Ashwani K.},
abstractNote = {We performed a comparative study of mode-selectivity of water dissociation on Ni(100), Ni(110), and Ni(111) surfaces at the same level of theory using a fully quantum approach based on the reaction path Hamiltonian. Calculations show that the barrier to water dissociation on the Ni(110) surface is significantly lower compared to its close-packed counterparts. Transition states for this reaction on all three surfaces involve the elongation of one of the O–H bonds. Furthermore, a significant decrease in the symmetric stretching and bending mode frequencies near the transition state is observed in all three cases and in the vibrational adiabatic approximation, excitation of these softened modes results in a significant enhancement in reactivity. Inclusion of non-adiabatic couplings between modes results in the asymmetric stretching mode showing a similar enhancement of reactivity as the symmetric stretching mode. Dissociation probabilities calculated at a surface temperature of 300 K showed higher reactivity at lower collision energies compared to that of the static surface case, underlining the importance of lattice motion in enhancing reactivity. Mode selective behavior is similar on all the surfaces. Molecules with one-quantum of vibrational excitation in the symmetric stretch, at lower energies (up to 0.45 eV), are more reactive on Ni(110) than the Ni(100) and Ni(111) surfaces. But, the dissociation probabilities approach saturation on all the surfaces at higher incident energy values. Ultimately, Ni(110) is found to be highly reactive toward water dissociation among the low-index nickel surfaces owing to a low reaction barrier resulting from the openness and corrugation of the surface. These results show that the mode-selective behavior does not vary with different crystal facets of Ni qualitatively, but there is a significant quantitative effect.},
doi = {10.1063/1.4976133},
journal = {Journal of Chemical Physics},
number = 7,
volume = 146,
place = {United States},
year = {2017},
month = {2}
}
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