Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures
The high pressure structural behavior of H<sub>2</sub> and Ne clathrate hydrates with approximate composition H<sub>2</sub>/Ne·~4H<sub>2</sub>O and featuring cubic structure II (CS-II) was investigated by neutron powder diffraction using the deuterated analogues a...
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MDPI AG
2021-12-01
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| Series: | Crystals |
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| Online Access: | https://www.mdpi.com/2073-4352/12/1/9 |
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| author | Paulo H. B. Brant Carvalho Amber Mace Inna Martha Nangoi Alexandre A. Leitão Chris A. Tulk Jamie J. Molaison Ove Andersson Alexander P. Lyubartsev Ulrich Häussermann |
| author_facet | Paulo H. B. Brant Carvalho Amber Mace Inna Martha Nangoi Alexandre A. Leitão Chris A. Tulk Jamie J. Molaison Ove Andersson Alexander P. Lyubartsev Ulrich Häussermann |
| author_sort | Paulo H. B. Brant Carvalho |
| collection | DOAJ |
| description | The high pressure structural behavior of H<sub>2</sub> and Ne clathrate hydrates with approximate composition H<sub>2</sub>/Ne·~4H<sub>2</sub>O and featuring cubic structure II (CS-II) was investigated by neutron powder diffraction using the deuterated analogues at ~95 K. CS-II hydrogen hydrate transforms gradually to isocompositional C<sub>1</sub> phase (filled ice II) at around 1.1 GPa but may be metastably retained up to 2.2 GPa. Above 3 GPa a gradual decomposition into C<sub>2</sub> phase (H<sub>2</sub>·H<sub>2</sub>O, filled ice I<sub>c</sub>) and ice VIII’ takes place. Upon heating to 200 K the CS-II to C<sub>1</sub> transition completes instantly whereas C<sub>1</sub> decomposition appears sluggish also at 200 K. C<sub>1</sub> was observed metastably up to 8 GPa. At 95 K C<sub>1</sub> and C<sub>2</sub> hydrogen hydrate can be retained below 1 GPa and yield ice II and ice I<sub>c</sub>, respectively, upon complete release of pressure. In contrast, CS-II neon hydrate undergoes pressure-induced amorphization at 1.9 GPa, thus following the general trend for noble gas clathrate hydrates. Upon heating to 200 K amorphous Ne hydrate crystallizes as a mixture of previously unreported C<sub>2</sub> hydrate and ice VIII’. |
| first_indexed | 2024-03-10T01:41:18Z |
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| issn | 2073-4352 |
| language | English |
| last_indexed | 2024-03-10T01:41:18Z |
| publishDate | 2021-12-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Crystals |
| spelling | doaj.art-5d07f04a826c4a8988ce2a10171c81122023-11-23T13:23:41ZengMDPI AGCrystals2073-43522021-12-01121910.3390/cryst12010009Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low TemperaturesPaulo H. B. Brant Carvalho0Amber Mace1Inna Martha Nangoi2Alexandre A. Leitão3Chris A. Tulk4Jamie J. Molaison5Ove Andersson6Alexander P. Lyubartsev7Ulrich Häussermann8Department of Materials and Environmental Chemistry, Stockholm University, SE-10691 Stockholm, SwedenDepartment of Chemistry-Ångström Laboratory, Uppsala University, SE-75236 Uppsala, SwedenDepartment of Chemistry, Federal University of Juiz de Fora, Juiz de Fora 36036-900, BrazilDepartment of Chemistry, Federal University of Juiz de Fora, Juiz de Fora 36036-900, BrazilNeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USANeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USADepartment of Physics, Umeå University, SE-90187 Umeå, SwedenDepartment of Materials and Environmental Chemistry, Stockholm University, SE-10691 Stockholm, SwedenDepartment of Materials and Environmental Chemistry, Stockholm University, SE-10691 Stockholm, SwedenThe high pressure structural behavior of H<sub>2</sub> and Ne clathrate hydrates with approximate composition H<sub>2</sub>/Ne·~4H<sub>2</sub>O and featuring cubic structure II (CS-II) was investigated by neutron powder diffraction using the deuterated analogues at ~95 K. CS-II hydrogen hydrate transforms gradually to isocompositional C<sub>1</sub> phase (filled ice II) at around 1.1 GPa but may be metastably retained up to 2.2 GPa. Above 3 GPa a gradual decomposition into C<sub>2</sub> phase (H<sub>2</sub>·H<sub>2</sub>O, filled ice I<sub>c</sub>) and ice VIII’ takes place. Upon heating to 200 K the CS-II to C<sub>1</sub> transition completes instantly whereas C<sub>1</sub> decomposition appears sluggish also at 200 K. C<sub>1</sub> was observed metastably up to 8 GPa. At 95 K C<sub>1</sub> and C<sub>2</sub> hydrogen hydrate can be retained below 1 GPa and yield ice II and ice I<sub>c</sub>, respectively, upon complete release of pressure. In contrast, CS-II neon hydrate undergoes pressure-induced amorphization at 1.9 GPa, thus following the general trend for noble gas clathrate hydrates. Upon heating to 200 K amorphous Ne hydrate crystallizes as a mixture of previously unreported C<sub>2</sub> hydrate and ice VIII’.https://www.mdpi.com/2073-4352/12/1/9hydrogen hydrateneon hydratepressure effectsneutron diffractionmolecular dynamicsclathrate hydrates |
| spellingShingle | Paulo H. B. Brant Carvalho Amber Mace Inna Martha Nangoi Alexandre A. Leitão Chris A. Tulk Jamie J. Molaison Ove Andersson Alexander P. Lyubartsev Ulrich Häussermann Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures Crystals hydrogen hydrate neon hydrate pressure effects neutron diffraction molecular dynamics clathrate hydrates |
| title | Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures |
| title_full | Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures |
| title_fullStr | Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures |
| title_full_unstemmed | Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures |
| title_short | Exploring High-Pressure Transformations in Low-Z (H<sub>2</sub>, Ne) Hydrates at Low Temperatures |
| title_sort | exploring high pressure transformations in low z h sub 2 sub ne hydrates at low temperatures |
| topic | hydrogen hydrate neon hydrate pressure effects neutron diffraction molecular dynamics clathrate hydrates |
| url | https://www.mdpi.com/2073-4352/12/1/9 |
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