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Elucidating the guest disorder in structure II argon hydrate: A neutron diffraction isotopic substitution study
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik.
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2020 (Engelska)Ingår i: Journal of Solid State Chemistry, ISSN 0022-4596, E-ISSN 1095-726X, Vol. 285, artikel-id 121220Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Clathrate hydrates with the cubic structure II (CS-II) form typically with large guest molecules, such as tetrahydrofuran, trimethylamine oxide, or propane. However, CS-II is also realized for argon hydrate despite the comparatively small van der Waals diameter of the guest (around 3.8 angstrom). Here, the structure of deuterated argon hydrate was studied at ambient pressure in the temperature range 20-95 K using neutron diffraction and comparing natural Ar with Ar-36, which scatters neutrons more than 13 times more efficiently. The procedure allowed to unambiguously establish the positional disorder within the large cages of CS-H, while simultaneously refining host and guest structures. These cages are singly occupied and off-centered argon atoms distribute on two tetrahedron-shaped split positions with a ratio 3:1. Molecular dynamics (MD) simulations revealed that the crystallographic positional disorder structure is due to mobile argon atoms even at 20 K. The MD potential energy distribution confirmed the diffraction model. It is noted that the unit cell volumes of argon hydrate in the investigated temperature range are virtually identical to N-2 hydrate, which has a similar composition at ambient pressure, indicating a very similar (slightly attractive) host-guest interaction.

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Elsevier, 2020. Vol. 285, artikel-id 121220
Nyckelord [en]
Clathrate hydrates, Disorder, Neutron diffraction
Nationell ämneskategori
Oorganisk kemi Materialkemi Den kondenserade materiens fysik
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URN: urn:nbn:se:umu:diva-169764DOI: 10.1016/j.jssc.2020.121220ISI: 000521107900003Scopus ID: 2-s2.0-85078663372OAI: oai:DiVA.org:umu-169764DiVA, id: diva2:1428996
Tillgänglig från: 2020-05-07 Skapad: 2020-05-07 Senast uppdaterad: 2023-03-24Bibliografiskt granskad

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Andersson, Ove

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