Intermetallic Compound AlPd As a Selective Hydrogenation Catalyst: A DFT Study

Author(s)
Marian Krajci, Juergen Hafner
Abstract

Recently, it has been demonstrated that intermetallic compounds composed of Pd and Ga or Co and Al provide excellent selectivity for the hydrogenation of acetylene to ethylene. Motivated by experimental works on GaPd catalysts, we have performed a detailed ab initio study of acetylene hydrogenation by the pseudo 5-fold (120) surface of the isostructural and isoelectronic AlPd compound crystallizing in the B20-type structure. The structure of the surface can be described by a triangle-rectangle tiling, and we demonstrate that the most active sites for hydrogenation are triangular arrangements of two Al and one Pd atom. Acetylene is bound to bridge sites between two Al atoms. The most favorable adsorption site for ethylene is on top of the most strongly protruding Pd atom. Activation energies for all steps of the reaction have been calculated. We demonstrate that the activation energies for the rate-controlling steps are comparable to those on reference catalysts (Pd, Pd-Ag and Al13Co4) and that a desorption energy for ethylene that is lower than the activation energy of ethylene to ethyl provides thus good selectivity. We show that the decisive factors for the activity and selectivity of the catalyst are the same on both intermetallic compounds AlPd and Al13Co4.

Organisation(s)
Computational Materials Physics
External organisation(s)
Slovenian Academy of Sciences and Arts
Journal
The Journal of Physical Chemistry Part C (Nanomaterials and Interfaces)
Volume
116
Pages
6307-6319
No. of pages
13
ISSN
1932-7447
DOI
https://doi.org/10.1021/jp212317u
Publication date
2012
Peer reviewed
Yes
Austrian Fields of Science 2012
103018 Materials physics
Portal url
https://ucrisportal.univie.ac.at/en/publications/intermetallic-compound-alpd-as-a-selective-hydrogenation-catalyst-a-dft-study(3e0df755-07bc-4f4a-ac3e-49e500792698).html