Kinetic Regimes in Ethylene Hydrogenation over Transition-Metal Surfaces
Journal article, 2016

A first-principles microkinetic model has been developed and applied to ethylene hydrogenation over close-packed transition-metal surfaces of Ru, Rh, Pd, Os, Ir, and Pt. The model is based on density functional theory calculations, which have been used to determine the activation energies of the elementary steps of the reaction according to the Horuiti-Polanyi mechanism. A sensitivity analysis of the activity with respect to the kinetic parameters reveals distinctly different kinetic regimes across the periodic table. For Ru and Ir, the activity is controlled by the activation energy for ethylene to ethyl hydrogenation, whereas the other metals also have a sensitivity to the second hydrogenation step. The analysis shows, furthermore, that the activity could be enhanced considerably with minor reductions of the hydrogenation barriers.

hydrogenation

DFT

ethylene

microkinetic modeling

transition metals

Author

Christopher Heard

Competence Centre for Catalysis (KCK)

Chalmers, Physics, Chemical Physics

Hu Chaoquan

Competence Centre for Catalysis (KCK)

Chalmers, Chemistry and Chemical Engineering, Chemical Technology

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Competence Centre for Catalysis (KCK)

Derek Creaser

Chalmers, Chemistry and Chemical Engineering, Chemical Technology

Competence Centre for Catalysis (KCK)

Henrik Grönbeck

Competence Centre for Catalysis (KCK)

Chalmers, Physics, Chemical Physics

ACS Catalysis

21555435 (eISSN)

Vol. 6 5 3277-3286

Areas of Advance

Transport

Subject Categories

Chemical Engineering

Theoretical Chemistry

DOI

10.1021/acscatal.5b02708

More information

Created

10/7/2017