The dehydrogenation of ethylene on Pd second-neighbor ensembles of both PdAu(1 0 0) and PdAu(1 1 1) surface alloys in presence of surface oxygen atoms (Os) and hydroxyl groups (OHs) was investigated at the density functional level with a cluster model approach. The calculated activation barriers for ethylene dehydrogenation to form vinyl on Os-and OHs-covered PdAu surfaces are significantly lower than those on clean surface alloys. Therefore, our outcomes suggest that a Langmuir-Hinshelwood-type mechanism involving a vinyl surface species cannot be excluded a priori when investigating the microscopic behaviour of the oxygen-assisted acetoxylation of ethylene on PdAu catalysts. © 2010 Elsevier B.V. All rights reserved.
The influence of surface oxygen and hydroxyl groups on the dehydrogenation of ethylene on PdAu surface alloys. A theoretical cluster model study / Rivalta, Ivan; Mazzone, Gloria; Russo, Nino; Sicilia, Emilia*. - In: CHEMICAL PHYSICS LETTERS. - ISSN 0009-2614. - STAMPA. - 493:1-3(2010), pp. 87-93. [10.1016/j.cplett.2010.05.033]
The influence of surface oxygen and hydroxyl groups on the dehydrogenation of ethylene on PdAu surface alloys. A theoretical cluster model study
Rivalta, Ivan;SICILIA, EMILIA MARIA GIUSEPPINA FRANC.
2010
Abstract
The dehydrogenation of ethylene on Pd second-neighbor ensembles of both PdAu(1 0 0) and PdAu(1 1 1) surface alloys in presence of surface oxygen atoms (Os) and hydroxyl groups (OHs) was investigated at the density functional level with a cluster model approach. The calculated activation barriers for ethylene dehydrogenation to form vinyl on Os-and OHs-covered PdAu surfaces are significantly lower than those on clean surface alloys. Therefore, our outcomes suggest that a Langmuir-Hinshelwood-type mechanism involving a vinyl surface species cannot be excluded a priori when investigating the microscopic behaviour of the oxygen-assisted acetoxylation of ethylene on PdAu catalysts. © 2010 Elsevier B.V. All rights reserved.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.