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A Second Glass Transition in Pressure Collapsed Type II Clathrate Hydrates
Umeå University, Faculty of Science and Technology, Department of Physics.
2018 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 122, no 15, p. 4376-4384Article in journal (Refereed) Published
Abstract [en]

Type II clathrate hydrates (CHs) M·17 H2O, with M = tetrahydrofuran (THF) or 1,3-dioxolane, are known to collapse, or amorphize, on pressurization to ∼1.3 GPa in the temperature range 77–140 K. On heating at 1 GPa, these pressure-amorphized CH states show a weak, stretched sigmoid-shaped, heat-capacity increase because of a glass transition. Here we use thermal conductivity and heat capacity measurements to show that also type II CH with M = cyclobutanone (CB) collapses on isothermal pressurization and undergoes a similar, weak, glass transition upon heating at 1 GPa. Furthermore, we reveal for both THF CH and CB CH a second, much more pronounced, glass transition at temperatures above the thermally weak glass transition on heating in the 0.2–0.7 GPa range. This result suggests the general occurrence of two glass transitions in water-rich (94 mol %) pressure-collapsed CHs. Because of a large increase in dielectric permittivity concurrently as the weak heat capacity increase, the first glass transition must be due to kinetic unfreezing of water molecules. The thermal features of the second glass transition, measured on isobaric temperature cycling, are typical of a glass–liquid–glass transition, which suggests that pressure-amorphized CHs transform reversibly to liquids.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 122, no 15, p. 4376-4384
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:umu:diva-151173DOI: 10.1021/acs.jpcb.8b01269ISI: 000430784000019PubMedID: 29584946Scopus ID: 2-s2.0-85045728560OAI: oai:DiVA.org:umu-151173DiVA, id: diva2:1245658
Conference
International Conference on NMR Spectroscopy of Biomolecules, APR 16-17, 2016, Univ Michigan, Ann Arbor, MI
Available from: 2018-09-05 Created: 2018-09-05 Last updated: 2018-09-05Bibliographically approved

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Andersson, Ove

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