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surface chemoselective, results from the addition of one H atom
to the CC bond of acrolein to form oxopropyl species. After
a dense overlayer of the spectator is formed, acrolein adsorbs
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selectively hydrogenated to an unsaturated alcohol propenol.
The nature of the corresponding surface reaction intermediate
was established spectroscopically. By monitoring the surface
species during the course of the reaction via IRAS, we were able
for the first time to experimentally follow the simultaneous
evolution of the reactive intermediate on the surface and
formation of the product in the gas phase. With this a direct
assignment of one of the surface species to a reaction
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by strong acrolein decarbonylation, and the surface was
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bond (Figure 5b).
Obtained atomistic-level insights into chemoselective hydro-
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the catalytically active surface under reaction conditions.
Related effects are expected to play a key role in controlling
chemoselectivity in hydrogenation of all types of α,β-
unsaturated aldehydes and ketones and hold a great potential
for further development of new chemo- and enantioselective
powdered catalysts such as e.g. ligand-modified nanoparticles.
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ASSOCIATED CONTENT
* Supporting Information
The Supporting Information is available free of charge on the
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Further details on the preparation procedure of
supported model catalysts, the scanning tunneling
microscopy image of the resulting surface, and more
detailed discussion on of the reactivity on Pd nano-
AUTHOR INFORMATION
Corresponding Author
Notes
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The authors declare no competing financial interest.
ACKNOWLEDGMENTS
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Support from the European Research Council (ERC Starting
Grant ENREMOS, project number 335205) is gratefully
acknowledged. S.S. thanks the Fonds der Chemischen Industrie
for the Chemiedozentenstipendium.
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