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Title: Degree of rate control approach to computational catalyst screening

Abstract

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 relationships 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 (<0.5 eV different on a plot where the axes are the bond energies to C and O adatoms), but worse when too different frommore » the reference. It is computationally faster than the NB method when screening a moderate number of materials (<100), thus adding a valuable complement to the NB approach. It can be implemented without a microkinetic model if the degrees of rate control are already known approximately, e.g., from experiments.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1370938
DOE Contract Number:  
SC0012702
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 330; Journal Issue: C; Related Information: ICDC partners with University of Minnesota(lead); Argonne National Laboratory; Clemson University; Dow Chemical Company; Northwestern University; Pacific Northwest National Laboratory; University of California Davis; University of Washington; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous), materials and chemistry by design, synthesis (novel materials)

Citation Formats

Wolcott, Christopher A., Medford, Andrew J., Studt, Felix, and Campbell, Charles T. Degree of rate control approach to computational catalyst screening. United States: N. p., 2015. Web. doi:10.1016/j.jcat.2015.07.015.
Wolcott, Christopher A., Medford, Andrew J., Studt, Felix, & Campbell, Charles T. Degree of rate control approach to computational catalyst screening. United States. doi:10.1016/j.jcat.2015.07.015.
Wolcott, Christopher A., Medford, Andrew J., Studt, Felix, and Campbell, Charles T. Thu . "Degree of rate control approach to computational catalyst screening". United States. doi:10.1016/j.jcat.2015.07.015.
@article{osti_1370938,
title = {Degree of rate control approach to computational catalyst screening},
author = {Wolcott, Christopher A. and Medford, Andrew J. and Studt, Felix and Campbell, Charles T.},
abstractNote = {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 relationships 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 (<0.5 eV different on a plot where the axes are the bond energies to C and O adatoms), but worse when too different from the reference. It is computationally faster than the NB method when screening a moderate number of materials (<100), thus adding a valuable complement to the NB approach. It can be implemented without a microkinetic model if the degrees of rate control are already known approximately, e.g., from experiments.},
doi = {10.1016/j.jcat.2015.07.015},
journal = {Journal of Catalysis},
issn = {0021-9517},
number = C,
volume = 330,
place = {United States},
year = {2015},
month = {10}
}