Degree of rate control approach to computational catalyst screening

Authors
Christopher A. Wolcott,
Andrew J. Medford,
Felix Studt,
Charles T. Campbell
Year of publication
2015
Journal
Journal of Catalysis
Volume
330
Starting page
197
Ending page
207
A new method for computational catalyst screening that is based on the concept of the degree of rate control (DRC) is introduced. It starts by developing a full mechanism and microkinetic model at the conditions of interest for a reference catalyst (ideally, the best known material) and then determines the degrees of rate control of the species in the mechanism (i.e., all adsorbed intermediates and transition states). It then uses the energies of the few species with the highest DRCs for this reference catalyst as descriptors to estimate the rates on related materials and predict which are most active. The predictions of this method regarding the relative rates of twelve late transition metals for methane steam reforming, using the Rh(2 1 1) surface as the reference catalyst, are compared to the most commonly-used approach for computation catalyst screening, the Nørskov–Bligaard (NB) method which uses linear scaling relation- ships to estimate the energies of all adsorbed intermediates and transition states. It is slightly more accurate than the NB approach when the metals are similar to the reference metal (
Keywords
Catalyst screening, Computational catalysis, Density functional theory, Degree of rate control
Funding sources