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| Main Authors: | , , , , , , , |
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| Format: | Preprint |
| Published: |
2025
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2502.08078 |
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| _version_ | 1866913687714922496 |
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| author | Huang, Yang Zhang, Le Ji, Hefei Zhang, Zhipeng Zhang, Qili Sun, Bo Liu, Haifeng Song, Haifeng |
| author_facet | Huang, Yang Zhang, Le Ji, Hefei Zhang, Zhipeng Zhang, Qili Sun, Bo Liu, Haifeng Song, Haifeng |
| contents | Unraveling the adsorption mechanism and thermodynamics of O$_2$ and H$_2$O on uranium dioxide surfaces is critical for the nuclear fuel storage and uranium corrosion. Based on the first-principles DFT+U-D3 calculations, we carefully test the effect of antiferromagnetic order arrangements on the thermodynamic stability of UO$_2$ surfaces and propose the 1k AFM surface computational model. The chemisorption states of O$_2$ and H$_2$O on UO$_2$ (111) surface, suggested by previous experiments, are accurately calculated for the first time. The adsorption properties of O$_2$ and H$_2$O on UO$_2$(111) and (110) surfaces are discussed in detail to reveal the different interaction mechanisms. Combined with ab initio atomistic thermodynamics method, we systematically calculate the chemisorption phase diagram and isotherm of O$_2$ and H$_2$O on UO$_2$ surfaces. Due to the different intermolecular interactions, the monolayer and multilayer adsorption models are identified for O$_2$ and H$_2$O, respectively. This study has comprehensively revealed the different adsorption mechanisms of O$_2$ and H$_2$O on UO$_2$ surfaces, bridging the electronic structure calculations to the interpretation of experimental results and providing a solid foundation for future theoretical studies of uranium corrosion mechanism in humid air. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2502_08078 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | The chemisorption thermodynamics of O$_2$ and H$_2$O on AFM UO$_2$ surfaces unraveled by DFT+U-D3 study Huang, Yang Zhang, Le Ji, Hefei Zhang, Zhipeng Zhang, Qili Sun, Bo Liu, Haifeng Song, Haifeng Materials Science Computational Physics Unraveling the adsorption mechanism and thermodynamics of O$_2$ and H$_2$O on uranium dioxide surfaces is critical for the nuclear fuel storage and uranium corrosion. Based on the first-principles DFT+U-D3 calculations, we carefully test the effect of antiferromagnetic order arrangements on the thermodynamic stability of UO$_2$ surfaces and propose the 1k AFM surface computational model. The chemisorption states of O$_2$ and H$_2$O on UO$_2$ (111) surface, suggested by previous experiments, are accurately calculated for the first time. The adsorption properties of O$_2$ and H$_2$O on UO$_2$(111) and (110) surfaces are discussed in detail to reveal the different interaction mechanisms. Combined with ab initio atomistic thermodynamics method, we systematically calculate the chemisorption phase diagram and isotherm of O$_2$ and H$_2$O on UO$_2$ surfaces. Due to the different intermolecular interactions, the monolayer and multilayer adsorption models are identified for O$_2$ and H$_2$O, respectively. This study has comprehensively revealed the different adsorption mechanisms of O$_2$ and H$_2$O on UO$_2$ surfaces, bridging the electronic structure calculations to the interpretation of experimental results and providing a solid foundation for future theoretical studies of uranium corrosion mechanism in humid air. |
| title | The chemisorption thermodynamics of O$_2$ and H$_2$O on AFM UO$_2$ surfaces unraveled by DFT+U-D3 study |
| topic | Materials Science Computational Physics |
| url | https://arxiv.org/abs/2502.08078 |