A benchmark database for adsorption bond energies to transition metal surfaces and comparison to selected DFT functionals

Wellendorff, Jess; Silbaugh, Trent L.; Garcia-Pintos, Delfina; Nørskov, Jens K.; Bligaard, Thomas; Studt, Felix; Campbell, Charles T.

doi:10.1016/j.susc.2015.03.023

Cited by 457 publications

(647 citation statements)

References 85 publications

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“…that included 10 chemisorption energies for CO adsorption and 8 energies for H 2 adsorption on different transition metals. However, Wellendorff et al . subsequently discovered that several of these energies had large calibration errors or were invalid and therefore they refined the tables and compiled an experimental database for 39 different adsorption reactions occurring on 10 different transition metal surfaces.…”

Section: Modelling Catalyst Surfacesmentioning

confidence: 57%

“…There is no well‐defined way to know what contribution to the adsorption energy really comes from van der Waals interactions and therefore it is not exactly know how to classify surface reactions into the two classes provided by Wellendorff et al . Different division of the experimental database was proposed by Duanmu et al .…”

Section: Modelling Catalyst Surfacesmentioning

confidence: 99%

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Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

et al. 2020

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Density functional theory (DFT) of the CO2 behavior on the catalyst surface provides valuable insights about the C=O bond activation, information about adsorption and dissociation of CO2, understanding the elementary steps involved in the mechanism of the CO2 hydrogenation reaction. Nowadays, DFT computational studies for the catalytic hydrogenation of CO2 are becoming very popular. Therefore, this article is focused on a comprehensive review of the DFT studies in thermocatalytic hydrogenation of CO2 at the gas‐surface interface and discusses three aspects: 1) processes taking place on the surfaces and facets of transition metal heterogeneous catalysts, 2) adsorption of CO2 on surfaces of different transition metals; 3) current understanding of reaction mechanisms taking place on the catalytic surface for the production of different compounds. A detailed schematic overview of the possible CO2 hydrogenation mechanisms and DFT simulations presented here will enhance the current understanding of the CO2 catalytic hydrogenation.

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Section: Modelling Catalyst Surfacesmentioning

confidence: 57%

Section: Modelling Catalyst Surfacesmentioning

confidence: 99%

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

et al. 2020

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“…In addition, for future studies, we think it would be beneficial to expand and improve the current training and validation datasets; by for example, using the dispersion dataset S66x8 instead of S22x5, 94 including more solid state systems, 95 and reevaluate the chemisorption dataset. 96 For developing more accurate BEEF functionals, we also need to address the self-interaction error. This could be done by either introducing (screened) exact exchange or by using a self-interaction correction scheme, such as Hubbard +U or SIC.…”

Section: Summary Discussion and Conclusionmentioning

confidence: 99%

mBEEF-vdW: Robust fitting of error estimation density functionals

et al. 2016

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We propose a new general-purpose semi-local/non-local exchange-correlation functional approximation, named mBEEF-vdW. The exchange is a meta-generalized gradient approximation, and the correlation is a semi-local and non-local mixture, with the Rutgers-Chalmers approximation for van der Waals forces. The functional is fitted within the Bayesian error estimation functional framework (2014)]. We improve the previously used fitting procedures by introducing a robust MM-estimator based loss function, reducing the sensitivity to outliers in the datasets. To more reliably determine the optimal model complexity, we furthermore introduce a generalization of the bootstrap 0.632 estimator with hierarchical bootstrap sampling and geometric mean estimator over the training datasets. Using this estimator, we show that the robust loss function leads to a 10% improvement in the estimated prediction error over the previously used least squares loss function. The mBEEF-vdW functional is benchmarked against popular density functional approximations over a wide range of datasets relevant for heterogeneous catalysis, including datasets that were not used for its training. Overall, we find that mBEEF-vdW has a higher general accuracy than competing popular functionals, and it's one of the best performing functionals on chemisorption systems, surface energies, lattice constants, and dispersion. We also show the potential energy curve of graphene on the nickel(111) surface, where mBEEF-vdW match the experimental binding length. mBEEF-vdW is currently available in GPAW and other DFT codes through LIBXC version 3.0.0.

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“…All calculations were performed using plane‐wave DFT employing Vanderbilt ultrasoft pseudopotentials . The QUANTUM ESPRESSO code and the BEEF‐vdW exchange correlation functional were used for all calculations utilizing that this particular functional shows good performance in describing oxygen/transition metal systems . The plane‐wave cutoff and density cutoff were 500 eV and 5000 eV, respectively.…”

Section: Computational Detailsmentioning

confidence: 99%

Methanol Partial Oxidation on Ag(1 1 1) from First Principles

et al. 2016

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In this work, we examine the thermochemistry and kinetics of the partial oxidation of methanol to formaldehyde on silver surfaces. Periodic density functional theory calculations employing the BEEF‐vdW functional are used to identify the most stable phases of the silver surface under relevant reaction conditions and the reaction energetics are obtained on these surfaces. The calculated binding energies and transition state energies are used as input in a mean‐field microkinetic model providing the reaction kinetics on silver surfaces under different reaction conditions. Our results show that, under conditions pertaining to methanol partial oxidation, oxygen is present at low concentrations and it plays a critical role in the catalytic reaction. Surface oxygen promotes the reaction by activating the OH bond in methanol, thus forming a methoxy intermediate, which can react further to form formaldehyde. The dissociation of molecular oxygen is identified as the most critical step.

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A benchmark database for adsorption bond energies to transition metal surfaces and comparison to selected DFT functionals

Cited by 457 publications

References 85 publications

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

mBEEF-vdW: Robust fitting of error estimation density functionals

Methanol Partial Oxidation on Ag(1 1 1) from First Principles

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A benchmark database for adsorption bond energies to transition metal surfaces and comparison to selected DFT functionals

Cited by 457 publications

References 85 publications

Recent Developments in the Modelling of Heterogeneous Catalysts for CO2 Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO2 Conversion to Chemicals

mBEEF-vdW: Robust fitting of error estimation density functionals

Methanol Partial Oxidation on Ag(1 1 1) from First Principles

Contact Info

Product

Resources

About

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals