Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces
Abstract
The quantitative prediction of adsorption energies of radicals and molecules on surfaces is essential for the design and understanding of heterogeneous catalytic processes. Here, a recent paper by Wellendorff et al. collected an experimental database of 39 reaction energies involving adsorption energies on transition metal surfaces that can be used as benchmarks for testing quantum mechanical electronic structure methods, and we compared the experimental data to Kohn–Sham density functional calculations with six exchange–correlation functionals. In this paper, we rearranged the data into two categories: open-shell radical adsorption reactions and closed-shell molecular adsorption reactions. We recalculated the adsorption energies with PBE, and we also calculated them with three functionals, M06-L, GAM, and MN15-L, that were not studied in the Wellendorff et al. paper; then we compared our results to the benchmark data. Of the nine functionals that have been compared to the databases, we find that BEEF-vdW, GAM, and RPBE perform best for the open-shell radical adsorption reactions, and MN15-L performs best for the closed-shell molecular adsorption, followed by BEEF-vdW and M06-L.
- Authors:
-
[1];
[2]
- Univ. of Minnesota, Minneapolis, MN (United States); Univ. of California, Los Angeles, CA (United States)
- Univ. of Minnesota, Minneapolis, MN (United States)
- 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)
- OSTI Identifier:
- 1388270
- Grant/Contract Number:
- SC0012702
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Theory and Computation
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 2; 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 1549-9618
- Publisher:
- American Chemical Society
- 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
Duanmu, Kaining, and Truhlar, Donald G. Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces. United States: N. p., 2016.
Web. doi:10.1021/acs.jctc.6b01156.
Duanmu, Kaining, & Truhlar, Donald G. Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces. United States. https://doi.org/10.1021/acs.jctc.6b01156
Duanmu, Kaining, and Truhlar, Donald G. Fri .
"Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces". United States. https://doi.org/10.1021/acs.jctc.6b01156. https://www.osti.gov/servlets/purl/1388270.
@article{osti_1388270,
title = {Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces},
author = {Duanmu, Kaining and Truhlar, Donald G.},
abstractNote = {The quantitative prediction of adsorption energies of radicals and molecules on surfaces is essential for the design and understanding of heterogeneous catalytic processes. Here, a recent paper by Wellendorff et al. collected an experimental database of 39 reaction energies involving adsorption energies on transition metal surfaces that can be used as benchmarks for testing quantum mechanical electronic structure methods, and we compared the experimental data to Kohn–Sham density functional calculations with six exchange–correlation functionals. In this paper, we rearranged the data into two categories: open-shell radical adsorption reactions and closed-shell molecular adsorption reactions. We recalculated the adsorption energies with PBE, and we also calculated them with three functionals, M06-L, GAM, and MN15-L, that were not studied in the Wellendorff et al. paper; then we compared our results to the benchmark data. Of the nine functionals that have been compared to the databases, we find that BEEF-vdW, GAM, and RPBE perform best for the open-shell radical adsorption reactions, and MN15-L performs best for the closed-shell molecular adsorption, followed by BEEF-vdW and M06-L.},
doi = {10.1021/acs.jctc.6b01156},
journal = {Journal of Chemical Theory and Computation},
number = 2,
volume = 13,
place = {United States},
year = {Fri Dec 16 00:00:00 EST 2016},
month = {Fri Dec 16 00:00:00 EST 2016}
}
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Works referencing / citing this record:
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