Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure
Abstract Gas hydrate mechanical stability under pressure is critically important in energy supply, global warming, and carbon-neutral technologies. The stability of these polyhedral guest–host crystals under increasing pressure is affected by host cage type and face connectivity as well as guest gas...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-02-01
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| Series: | Scientific Reports |
| Online Access: | https://doi.org/10.1038/s41598-023-29194-8 |
| _version_ | 1828041739614552064 |
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| author | Xiaodan Zhu André Guerra Phillip Servio Alejandro D. Rey |
| author_facet | Xiaodan Zhu André Guerra Phillip Servio Alejandro D. Rey |
| author_sort | Xiaodan Zhu |
| collection | DOAJ |
| description | Abstract Gas hydrate mechanical stability under pressure is critically important in energy supply, global warming, and carbon-neutral technologies. The stability of these polyhedral guest–host crystals under increasing pressure is affected by host cage type and face connectivity as well as guest gas occupancy. The geometry-imposed cage connectivity generates crystal lattices that include inclusion-matrix material composite structures. In this paper, we integrate Density Functional Theory simulations with a polyhedral-inspired composite material model that quantifies stability limits, failure modes, and the impact of the type of cage occupancy. DFT reveals the existence of two failure mechanisms under increasing pressure: (i) a multistep lattice breakdown under total occupancy and under only large cage occupancy and (ii) a single-step breakdown under zero occupancy as well as with only small cage occupancy. The DFT-composite model predicts optimal occupancy pathways to generate strength and critical occupancy pathways to promote decomposition. |
| first_indexed | 2024-04-10T17:19:26Z |
| format | Article |
| id | doaj.art-71f701cb3bb34651ba07a09f91a0976b |
| institution | Directory Open Access Journal |
| issn | 2045-2322 |
| language | English |
| last_indexed | 2024-04-10T17:19:26Z |
| publishDate | 2023-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj.art-71f701cb3bb34651ba07a09f91a0976b2023-02-05T12:09:17ZengNature PortfolioScientific Reports2045-23222023-02-0113111110.1038/s41598-023-29194-8Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressureXiaodan Zhu0André Guerra1Phillip Servio2Alejandro D. Rey3Department of Chemical Engineering, McGill UniversityDepartment of Chemical Engineering, McGill UniversityDepartment of Chemical Engineering, McGill UniversityDepartment of Chemical Engineering, McGill UniversityAbstract Gas hydrate mechanical stability under pressure is critically important in energy supply, global warming, and carbon-neutral technologies. The stability of these polyhedral guest–host crystals under increasing pressure is affected by host cage type and face connectivity as well as guest gas occupancy. The geometry-imposed cage connectivity generates crystal lattices that include inclusion-matrix material composite structures. In this paper, we integrate Density Functional Theory simulations with a polyhedral-inspired composite material model that quantifies stability limits, failure modes, and the impact of the type of cage occupancy. DFT reveals the existence of two failure mechanisms under increasing pressure: (i) a multistep lattice breakdown under total occupancy and under only large cage occupancy and (ii) a single-step breakdown under zero occupancy as well as with only small cage occupancy. The DFT-composite model predicts optimal occupancy pathways to generate strength and critical occupancy pathways to promote decomposition.https://doi.org/10.1038/s41598-023-29194-8 |
| spellingShingle | Xiaodan Zhu André Guerra Phillip Servio Alejandro D. Rey Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure Scientific Reports |
| title | Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure |
| title_full | Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure |
| title_fullStr | Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure |
| title_full_unstemmed | Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure |
| title_short | Atomistic-geometric simulations to investigate the mechanical stability of monocrystalline sI methane hydrates under pressure |
| title_sort | atomistic geometric simulations to investigate the mechanical stability of monocrystalline si methane hydrates under pressure |
| url | https://doi.org/10.1038/s41598-023-29194-8 |
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