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Controlling Ethylene Hydrogenation Reactivity on Pt 13 Clusters by Varying the Stoichiometry of the Amorphous Silica Support
Author(s) -
Crampton Andrew S.,
Rötzer Marian D.,
Schweinberger Florian F.,
Yoon Bokwon,
Landman Uzi,
Heiz Ueli
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201603332
Subject(s) - stoichiometry , ethylene , reactivity (psychology) , amorphous solid , catalysis , silicon , cluster (spacecraft) , selectivity , materials science , amorphous silicon , amorphous silica , chemistry , crystallography , chemical engineering , crystalline silicon , organic chemistry , medicine , alternative medicine , pathology , computer science , programming language , engineering
Ethylene hydrogenation was investigated on size‐selected Pt 13 clusters supported on three amorphous silica (a‐SiO 2 ) thin films with different stoichiometries. Activity measurements of the reaction at 300 K revealed that on a silicon‐rich and a stoichiometric film, Pt 13 exhibits a similar activity to that of Pt(111), in line with the known structure insensitivity of the reaction. On an oxygen‐rich film, a threefold increased rate was measured. Pulsing ethylene at 400 K, then measuring the activity at 300 K, resulted in complete loss of activity on the silicon‐rich surface compared to only marginal losses on the other surfaces. The measured reactivity trends correlate with charging characteristics of a Pt 13 cluster on the SiO 2 films, predicted through first‐principle calculations. The results reveal that the stoichiometry‐dependent charging by the support can be used to tune the selectivity of reaction pathways during a catalytic hydrogenation reaction.