Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces

Duanmu, Kaining; Truhlar, Donald G.

doi:10.1021/acs.jctc.6b01156

Title: Validation of Density Functionals for Adsorption Energies on Transition Metal Surfaces

Journal Article · Fri Dec 16 00:00:00 EST 2016 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.6b01156· OSTI ID:1388270

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Univ. of Minnesota, Minneapolis, MN (United States); Univ. of California, Los Angeles, CA (United States)
Univ. of Minnesota, Minneapolis, MN (United States)

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012702

OSTI ID:: 1388270

Journal Information:: Journal of Chemical Theory and Computation, Vol. 13, 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; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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Implicit solvent effects in the determination of Brønsted–Evans–Polanyi relationships for heterogeneously catalyzed reactions Gomes, José R. B.; Viñes, Francesc; Illas, Francesc Physical Chemistry Chemical Physics, Vol. 21, Issue 32 https://doi.org/10.1039/c9cp02817j	journal	January 2019
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Performance of density functionals for the structure and energetics of (M–O) ^0,± (M=Al, Si, Sc–Zn) Sampathkumar, Suresh; Paranthaman, Selvarengan Molecular Simulation, Vol. 45, Issue 6 https://doi.org/10.1080/08927022.2018.1557331	journal	December 2018
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