The structure of CO2 hydrate between 0.7 and 1.0 GPa

Tulk, Chris A.; Machida, Shinichi; Klug, Dennis D.; Lu, H.; Guthrie, Malcolm; Molaison, Jamie J.

doi:10.1063/1.4899265

Title: The structure of CO₂ hydrate between 0.7 and 1.0 GPa

Journal Article · Tue Nov 04 23:00:00 EST 2014 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.4899265 · OSTI ID:1286804

Tulk, Chris A. ^[1]; Machida, Shinichi ^[2]; Klug, Dennis D. ^[3]; Lu, H. ^[3]; Guthrie, Malcolm ^[4]; Molaison, Jamie J. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Science Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Science Division; Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.
National Research Council of Canada (NRC), Ottawa, ON (Canada)
Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.

A deuterated sample of CO₂ structure I (sI) clathrate hydrate (CO₂ ∙ 8.3 D₂O) has been formed and neutron diffraction experiments up to 1.0 GPa at 240 K were performed. The sI CO₂ hydrate transformed at 0.7 GPa into the high pressure phase that had been observed previously by Hirai, et al. (J. Phys. Chem. 133, 124511 (2010)) and O. Bollengier et al. (Geochim. Cosmochim. AC. 119, 322 (2013)), but which had not been structurally identified. The current neutron diffraction data were successfully fitted to a filled ice structure with CO₂ molecules filling the water channels. This CO₂+water system has also been investigated using classical molecular dynamics and density functional ab initio methods to provide additional characterization of the high pressure structure. Both models indicate the water network adapts an MH-III ‘like’ filled ice structure with considerable disorder of the orientations of the CO₂molecule. Furthermore, the disorder appears be a direct result of the level of proton disorder in the water network. In contrast to the conclusions of Bollengier et al. our neutron diffraction data shows that the filled ice phase can be recovered to ambient pressure (0.1 MPa) at 96 K, and recrystallization to sI hydrate occurs upon subsequent heating to 150 K, possibly by first forming low density amorphous ice. Unlike other clathrate hydrate systems, which transform from the sI or sII structure to the hexagonal structure (sH) then to the filled ice structure, CO₂ hydrate transforms directly from the sI form to the filled ice structure.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725; SC0001057

OSTI ID:: 1286804

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 17 Vol. 141; ISSN JCPSA6; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Water-carbon dioxide solid phase equilibria at pressures above 4 GPa Abramson, E. H.; Bollengier, O.; Brown, J. M. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-00915-0	journal	April 2017
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