Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys
Abstract The chemisorption energy is an integral aspect of surface chemistry, central to numerous fields such as catalysis, corrosion, and nanotechnology. Electronic-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surf...
| Main Authors: | , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2022-08-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-022-00846-z |
| _version_ | 1811342835058737152 |
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| author | Shikha Saini Joakim Halldin Stenlid Frank Abild-Pedersen |
| author_facet | Shikha Saini Joakim Halldin Stenlid Frank Abild-Pedersen |
| author_sort | Shikha Saini |
| collection | DOAJ |
| description | Abstract The chemisorption energy is an integral aspect of surface chemistry, central to numerous fields such as catalysis, corrosion, and nanotechnology. Electronic-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surfaces with optimal properties. However, existing methods are inadequate for interpreting complex, multi-metallic systems. Herein, we introduce a physics-based chemisorption model for alloyed transition metal surfaces employing primarily metal d-band properties that accounts for perturbations in both the substrate and adsorbate electronic states upon interaction. Importantly, we show that adsorbate-induced changes in the adsorption site interact with its chemical environment leading to a second-order response in chemisorption energy with the d-filling of the neighboring atoms. We demonstrate the robustness of the model on a wide range of transition metal alloys with O, N, CH, and Li adsorbates yielding a mean absolute error of 0.13 eV versus density functional theory reference chemisorption energies. |
| first_indexed | 2024-04-13T19:19:03Z |
| format | Article |
| id | doaj.art-6569b97b2d354bfc898719bdaba82e1a |
| institution | Directory Open Access Journal |
| issn | 2057-3960 |
| language | English |
| last_indexed | 2024-04-13T19:19:03Z |
| publishDate | 2022-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Computational Materials |
| spelling | doaj.art-6569b97b2d354bfc898719bdaba82e1a2022-12-22T02:33:36ZengNature Portfolionpj Computational Materials2057-39602022-08-018111210.1038/s41524-022-00846-zElectronic structure factors and the importance of adsorbate effects in chemisorption on surface alloysShikha Saini0Joakim Halldin Stenlid1Frank Abild-Pedersen2SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford UniversitySUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford UniversitySUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator LaboratoryAbstract The chemisorption energy is an integral aspect of surface chemistry, central to numerous fields such as catalysis, corrosion, and nanotechnology. Electronic-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surfaces with optimal properties. However, existing methods are inadequate for interpreting complex, multi-metallic systems. Herein, we introduce a physics-based chemisorption model for alloyed transition metal surfaces employing primarily metal d-band properties that accounts for perturbations in both the substrate and adsorbate electronic states upon interaction. Importantly, we show that adsorbate-induced changes in the adsorption site interact with its chemical environment leading to a second-order response in chemisorption energy with the d-filling of the neighboring atoms. We demonstrate the robustness of the model on a wide range of transition metal alloys with O, N, CH, and Li adsorbates yielding a mean absolute error of 0.13 eV versus density functional theory reference chemisorption energies.https://doi.org/10.1038/s41524-022-00846-z |
| spellingShingle | Shikha Saini Joakim Halldin Stenlid Frank Abild-Pedersen Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys npj Computational Materials |
| title | Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| title_full | Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| title_fullStr | Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| title_full_unstemmed | Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| title_short | Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| title_sort | electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys |
| url | https://doi.org/10.1038/s41524-022-00846-z |
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