Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
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A simple formulation of a generalized gradient approximation for the exchange and correlation energy of electrons has been proposed by Perdew, Burke, and Ernzerhof (PBE) [Phys. Rev. Lett. 77, 3865 (1996)]. Subsequently Zhang and Yang [Phys. Rev. Lett. 80, 890 (1998)] have shown that a slight revision of the PBE functional systematically improves the atomization energies for a large database of small molecules. In the present work, we show that the Zhang and Yang functional (revPBE) also improves the chemisorption energetics of atoms and molecules on transition-metal surfaces. Our test systems comprise atomic and molecular adsorption of oxygen, CO, and NO on Ni(100), Ni(111), Rh(100), Pd(100), and Pd(111) surfaces. As the revPBE functional may locally violate the Lieb-Oxford criterion, we further develop an alternative revision of the PBE functional, RPBE, which gives the same improvement of the chemisorption energies as the revPBE functional at the same time as it fulfills the Lieb-Oxford criterion locally.
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The RPBE exchange functional and van der Waals correction used in this study were previously shown to yield good agreement with experiments in terms of energetics and electronic structure for similar gas adsorption on an organometallic system.
“We used the RPBE exchange functional,22,23 and the van der Waals (vdW) correction24 which were previously shown to yield a good agreement with experiments in terms of energetics and electronic structure for similar gas adsorption on an organometallic system.25”
From Single-atom catalysts for CO <sub>2</sub> electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [22]
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Kim, M., Kim, S., Park, J., Lee, S., Jang, I., Kim, S., Lee, C. Y., Kwon, O. J., Ham, H. C., Hupp, J. T., et al. (2023) · Advanced Functional Materials · doi:10.1002/adfm.202300673 · Cited by 34 · see citing works
Phu, T. K. C., Hong, W. T., Han, H., Song, Y. I., Kim, J. H., Roh, S. H., Kim, M.-C., Koh, J. H., Oh, B.-K., Kim, J. Y., et al. (2024) · Materials Today · doi:10.1016/j.mattod.2024.05.007 · Cited by 22 · see citing works
Montenegro-Pohlhammer, N., Kuppusamy, S. K., Cárdenas-Jirón, G., Calzado, C. J., & Ruben, M. (2023) · Dalton Transactions · doi:10.1039/d2dt02598a · Cited by 11 · see citing works
- Authors
- Hammer, B., Hansen, L. B., & Nørskov, J. K.
- Affiliations
- Aalborg University (DK)
- Venue
- Physical Review B
- Publisher
- American Physical Society (APS)
- Published
- 1999-03-15
- Volume
- 59
- Issue
- 11
- Pages
- 7413-7421
- ISSN
- 0163-1829 (ISSN-L)
- 1095-3795
- OpenAlex
- W1991149034
- Cited by
- 8,270
- References
- 49
- Citations by year
- 2026: 549 · 2025: 744 · 2024: 706 · 2023: 548 · 2022: 594 · 2021: 528 · 2020: 488 · 2019: 416 · 2018: 347 · 2017: 296 · 2016: 311 · 2015: 279 · 2014: 264 · 2013: 263 · 2012: 241
- FWCI
- 33.12
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Physical review. B, Condensed matter (publishedVersion)
- Technical University of Denmark, DTU Orbit (Technical University of Denmark, DTU) (submittedVersion, other-oa)
- VBN Forskningsportal (Aalborg Universitet) (submittedVersion)
- Funders
- National Research Foundation
- Danmarks Grundforskningsfond
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Advanced Chemical Physics Studies
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Surface and Thin Film Phenomena
- Keywords
- generalized gradient approximation, exchange-correlation energy, adsorption energetics, chemisorption, transition metal surfaces, Ni(100), Ni(111), Rh(100), Pd(100), Pd(111), oxygen adsorption, CO adsorption, NO adsorption, atomization energies
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