Anomalous dynamics during sI to sII phase transformation in methane hydrate

DOI

Methane hydrate (MH) is a non-stoichiometric inclusion compound encaging CH4 molecules in a framework of H-bonded water molecules. It has attracted considerable attention over the past decade both for its geophysical relevancy and for its possible energy and environmental applications. Pressure is a key parameter in the study of this system as it induces substantial variations in the size of the cages as well as complete structural rearrangements. However, up to date, only structural and vibrational studies have been carried on high pressure MH, while no information is available on the guest molecule self-dynamics in the different HP polymorphs. In a recent QENS experiment using the HP Paris-Edinburgh apparatus, we unexpectedly observed a clear diffusive dynamics of methane molecules during the sI-sII phase transition. This anomalous dynamics could be linked to the existence of a high-mobility disordered layer between sI and sII coexistence regions [1,2]. Here we propose to shed light on the origin of this motion by measuring the QENS signal of a much larger volume sample (0.5 cm3 of methane hydrate CH4:D2O) contained in a standard HP piston cylinder device, in the 1-5 kbar range.

Identifier
DOI https://doi.org/10.5291/ILL-DATA.7-02-161
Metadata Access https://data.ill.fr/openaire/oai?verb=GetRecord&metadataPrefix=oai_datacite&identifier=10.5291/ILL-DATA.7-02-161
Provenance
Creator Ollivier, Jacques; Bove, Livia Eleonora; Koza, Michael Marek; Gaal, Richard; Klotz, Stefan; Ranieri, Umbertoluca; Kuhs, Werner Friedrich
Publisher Institut Laue-Langevin
Publication Year 2015
Rights OpenAccess; info:eu-repo/semantics/openAccess
OpenAccess true
Representation
Resource Type Dataset
Size 32 GB
Version 1
Discipline Particles, Nuclei and Fields