Adsorption energies are necessary but not sufficient to identify good catalysts
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| Autores principales: | , , , , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2025
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| _version_ | 1866908695203414016 |
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| author | Chatterjee, Shahana Davis, Alexander Podina, Lena Sharma, Divya Bengio, Yoshua Duval, Alexandre Voznyy, Oleksandr Hernández-Garcia, Alex Rolnick, David Therrien, Félix |
| author_facet | Chatterjee, Shahana Davis, Alexander Podina, Lena Sharma, Divya Bengio, Yoshua Duval, Alexandre Voznyy, Oleksandr Hernández-Garcia, Alex Rolnick, David Therrien, Félix |
| contents | As a core technology for green chemical synthesis and electrochemical energy storage, electrocatalysis is central to decarbonization strategies aimed at combating climate change. In this context, computational and machine learning driven catalyst discovery has emerged as a major research focus. These approaches frequently use the thermodynamic overpotential, calculated from adsorption free energies of reaction intermediates, as a key parameter in their analysis. In this paper, we explore the large-scale applicability of such overpotential estimates for identifying good catalyst candidates by using datasets from the Open Catalyst Project (OC20 and OC22). We start by quantifying the uncertainty in predicting adsorption energies using \textit{ab initio} methods and find that $\sim$0.3-0.5 eV is a conservative estimate for a single adsorption energy prediction. We then compute the overpotential of all materials in the OC20 and OC22 datasets for the hydrogen and oxygen evolution reactions. We find that while the overpotential allows the identification of known good catalysts such as platinum and iridium oxides, the uncertainty is large enough to misclassify a broad fraction of the datasets as ``good'', which limits its value as a screening criterion. These results question the reliance on overpotential estimation as a primary evaluation metric to sort through catalyst candidates and calls for a shift in focus in the computational catalysis and machine learning communities towards other metrics such as synthesizability, stability, lifetime or affordability. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_05938 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Adsorption energies are necessary but not sufficient to identify good catalysts Chatterjee, Shahana Davis, Alexander Podina, Lena Sharma, Divya Bengio, Yoshua Duval, Alexandre Voznyy, Oleksandr Hernández-Garcia, Alex Rolnick, David Therrien, Félix Materials Science Chemical Physics As a core technology for green chemical synthesis and electrochemical energy storage, electrocatalysis is central to decarbonization strategies aimed at combating climate change. In this context, computational and machine learning driven catalyst discovery has emerged as a major research focus. These approaches frequently use the thermodynamic overpotential, calculated from adsorption free energies of reaction intermediates, as a key parameter in their analysis. In this paper, we explore the large-scale applicability of such overpotential estimates for identifying good catalyst candidates by using datasets from the Open Catalyst Project (OC20 and OC22). We start by quantifying the uncertainty in predicting adsorption energies using \textit{ab initio} methods and find that $\sim$0.3-0.5 eV is a conservative estimate for a single adsorption energy prediction. We then compute the overpotential of all materials in the OC20 and OC22 datasets for the hydrogen and oxygen evolution reactions. We find that while the overpotential allows the identification of known good catalysts such as platinum and iridium oxides, the uncertainty is large enough to misclassify a broad fraction of the datasets as ``good'', which limits its value as a screening criterion. These results question the reliance on overpotential estimation as a primary evaluation metric to sort through catalyst candidates and calls for a shift in focus in the computational catalysis and machine learning communities towards other metrics such as synthesizability, stability, lifetime or affordability. |
| title | Adsorption energies are necessary but not sufficient to identify good catalysts |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2512.05938 |