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The first measurement of an absolute surface concentration of reaction intermediates in ethylene hydrogenation
Authors:Paul S. Cremer  Xingcai Su  Y. Ron Shen  Gabor A. Somorjai
Affiliation:(1) Materials Sciences Division, Lawrence Berkeley National Laboratories, University of California, 94720 Berkeley, CA, USA;(2) Department of Chemistry, University of California, 94720 Berkeley, CA, USA;(3) Department of Physics, University of California, 94720 Berkeley, CA, USA
Abstract:The first measurement of a turnover rate with respect to surface intermediate concentration in a high pressure heterogeneous catalytic reaction is reported. By using infrared-visible sum frequency generation to study the hydrogenation of ethylene on Pt(111), it was found that the surface concentration of pgr-bonded ethylene, the key reaction intermediate, represented approximately 4% of a monolayer. Thus the absolute turnover rate per surface adsorbed ethylene molecule is 25 times faster than the rate measured per platinum atom. To explain these results, we propose a model of weakly adsorbed ethylene intermediates reacting on atop sites.
Keywords:absolute surface intermediate concentration  ethylene hydrogenation  reaction intermediates in catalysis
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