The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations
Density functional theory (DFT) calculations are employed to study the oxygen evolution reaction (OER) on the edges of stripes of monolayer molybdenum disulfide. Experimentally, this material has been shown to evolve oxygen, albeit with low efficiency. Previous DFT studies have traced this low catal...
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| Format: | Article |
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MDPI AG
2023-07-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/28/13/5182 |
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| author | Estefania German Ralph Gebauer |
| author_facet | Estefania German Ralph Gebauer |
| author_sort | Estefania German |
| collection | DOAJ |
| description | Density functional theory (DFT) calculations are employed to study the oxygen evolution reaction (OER) on the edges of stripes of monolayer molybdenum disulfide. Experimentally, this material has been shown to evolve oxygen, albeit with low efficiency. Previous DFT studies have traced this low catalytic performance to the unfavourable adsorption energies of some reaction intermediates on the MoS<sub>2</sub> edge sites. In this work, we study the effects of the aqueous liquid surrounding the active sites. A computational approach is used, where the solvent is modeled as a continuous medium providing a dielectric embedding of the catalyst and the reaction intermediates. A description at this level of theory can have a profound impact on the studied reactions: the calculated overpotential for the OER is lowered from 1.15 eV to 0.77 eV. It is shown that such variations in the reaction energetics are linked to the polar nature of the adsorbed intermediates, which leads to changes in the calculated electronic charge density when surrounded by water. These results underline the necessity to computationally account for solvation effects, especially in aqueous environments and when highly polar intermediates are present. |
| first_indexed | 2024-03-11T01:33:38Z |
| format | Article |
| id | doaj.art-ca15ed15c55042ea8aa90d430294068f |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-11T01:33:38Z |
| publishDate | 2023-07-01 |
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| series | Molecules |
| spelling | doaj.art-ca15ed15c55042ea8aa90d430294068f2023-11-18T17:09:25ZengMDPI AGMolecules1420-30492023-07-012813518210.3390/molecules28135182The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular SimulationsEstefania German0Ralph Gebauer1Department of Theoretical, Atomic and Optical Physics, University of Valladolid, 47011 Valladolid, SpainThe Abdus Salam International Centre for Theoretical Physics (ICTP), Strada Costiera 11, 34151 Trieste, ItalyDensity functional theory (DFT) calculations are employed to study the oxygen evolution reaction (OER) on the edges of stripes of monolayer molybdenum disulfide. Experimentally, this material has been shown to evolve oxygen, albeit with low efficiency. Previous DFT studies have traced this low catalytic performance to the unfavourable adsorption energies of some reaction intermediates on the MoS<sub>2</sub> edge sites. In this work, we study the effects of the aqueous liquid surrounding the active sites. A computational approach is used, where the solvent is modeled as a continuous medium providing a dielectric embedding of the catalyst and the reaction intermediates. A description at this level of theory can have a profound impact on the studied reactions: the calculated overpotential for the OER is lowered from 1.15 eV to 0.77 eV. It is shown that such variations in the reaction energetics are linked to the polar nature of the adsorbed intermediates, which leads to changes in the calculated electronic charge density when surrounded by water. These results underline the necessity to computationally account for solvation effects, especially in aqueous environments and when highly polar intermediates are present.https://www.mdpi.com/1420-3049/28/13/5182oxygen evolution reactionwater splittingdensity functional theoryimplicit solventMoS<sub>2</sub>molybdenum disulfide |
| spellingShingle | Estefania German Ralph Gebauer The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations Molecules oxygen evolution reaction water splitting density functional theory implicit solvent MoS<sub>2</sub> molybdenum disulfide |
| title | The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations |
| title_full | The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations |
| title_fullStr | The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations |
| title_full_unstemmed | The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations |
| title_short | The Oxygen Evolution Reaction at MoS<sub>2</sub> Edge Sites: The Role of a Solvent Environment in DFT-Based Molecular Simulations |
| title_sort | oxygen evolution reaction at mos sub 2 sub edge sites the role of a solvent environment in dft based molecular simulations |
| topic | oxygen evolution reaction water splitting density functional theory implicit solvent MoS<sub>2</sub> molybdenum disulfide |
| url | https://www.mdpi.com/1420-3049/28/13/5182 |
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