Practical and accurate density functionals for transition-metal heterogeneous catalysis
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arXiv
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| Auteurs principaux: | , |
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| Format: | Preprint |
| Publié: |
2026
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| _version_ | 1866908902541492224 |
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| author | Shi, Benjamin X. Berkelbach, Timothy C. |
| author_facet | Shi, Benjamin X. Berkelbach, Timothy C. |
| contents | Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in rational catalyst design. These applications require reliable density functionals, however achieving transition-metal chemical accuracy (13 kJ/mol) on these properties remains challenging. We introduce a framework for designing new functionals tailored to catalytic processes on transition-metal surfaces, building on recent non-self-consistent approaches. Within this framework, we develop a hybrid and a double-hybrid functional that achieve unprecedented accuracy, with the latter reaching transition-metal chemical accuracy on average across 39 experimental adsorption reactions. In addition, both functionals demonstrate balanced performance for 17 barrier heights and correct qualitative failures of standard functionals, including CO adsorption on Pt(111) and graphene on Ni(111). They are computationally efficient, readily integrated into existing DFT codes, and supported by open-source workflows to facilitate adoption. More broadly, this framework provides a systematic route towards improved functionals for heterogeneous catalysis and complex materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_14962 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Practical and accurate density functionals for transition-metal heterogeneous catalysis Shi, Benjamin X. Berkelbach, Timothy C. Materials Science Chemical Physics Computational Physics Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in rational catalyst design. These applications require reliable density functionals, however achieving transition-metal chemical accuracy (13 kJ/mol) on these properties remains challenging. We introduce a framework for designing new functionals tailored to catalytic processes on transition-metal surfaces, building on recent non-self-consistent approaches. Within this framework, we develop a hybrid and a double-hybrid functional that achieve unprecedented accuracy, with the latter reaching transition-metal chemical accuracy on average across 39 experimental adsorption reactions. In addition, both functionals demonstrate balanced performance for 17 barrier heights and correct qualitative failures of standard functionals, including CO adsorption on Pt(111) and graphene on Ni(111). They are computationally efficient, readily integrated into existing DFT codes, and supported by open-source workflows to facilitate adoption. More broadly, this framework provides a systematic route towards improved functionals for heterogeneous catalysis and complex materials. |
| title | Practical and accurate density functionals for transition-metal heterogeneous catalysis |
| topic | Materials Science Chemical Physics Computational Physics |
| url | https://arxiv.org/abs/2602.14962 |