CO[subscript 2] hydrogenation to formic acid on Ni(111)
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revised-CO2-Ni111-subm-GP+MM.pdf
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Author(s)
Peng, Guowen
Sibener, S. J.
Schatz, George C.
Mavrikakis, Manos
Ceyer, Sylvia
Date Issued
December 2011
Journal
Journal of Physical Chemistry C
Publisher
American Chemical Society (ACS)
Citation
Peng, Guowen, S. J. Sibener, George C. Schatz, Sylvia T. Ceyer, and Manos Mavrikakis. “ CO[subscript 2] Hydrogenation to Formic Acid on Ni(111) .” The Journal of Physical Chemistry C 116, no. 4 (February 2, 2012): 3001–3006.
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Author's final manuscript
Abstract
Periodic, self-consistent, density functional theory (DFT) calculations are employed to study CO[subscript 2] hydrogenation on Ni(111). CO[subscript 2] hydrogenation with H adsorbed on the surface and with H absorbed in the subsurface is investigated systematically, and the respective microscopic reaction mechanisms are elucidated. We show that on Ni(111) CO[subscript 2] hydrogenation to formate intermediate is more favorable than to carboxyl intermediate. The hydrogenation to formate goes through the unidentate structure that rapidly transforms into the bidentate structure. Further hydrogenation from formate to formic acid is energetically more difficult than formate formation. Formation of adsorbed formic acid from adsorbed CO[subscript 2] and surface hydrogen is an endothermic reaction. Because subsurface H in Ni(111) is substantially less stable compared to surface H, its reaction with adsorbed CO[subscript 2] to adsorbed formic acid is an exothermic one. Our results may have significant implications for the synthesis of liquid fuels from CO[subscript 2] and for catalytic hydrogenation reactions in general.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/jp210408x
