Hydrogen in porous tetrahydrofuran clathrate hydrate

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dc.contributor.authorMulder, FMen_AU
dc.contributor.authorWagemaker, Men_AU
dc.contributor.authorvan Eijck, Len_AU
dc.contributor.authorKearley, GJen_AU
dc.date.accessioned2009-06-11T02:11:07Zen_AU
dc.date.accessioned2010-04-30T05:03:50Zen_AU
dc.date.available2009-06-11T02:11:07Zen_AU
dc.date.available2010-04-30T05:03:50Zen_AU
dc.date.issued2008-06-23en_AU
dc.date.statistics2008-06-23en_AU
dc.description.abstractThe lack of practical methods for hydrogen storage is still a major bottleneck in the realization of an energy economy based on hydrogen as energy carrier.([1]) Storage within solid-state clathrate hydrates,([2-4]) and in the clathrote hydrate of tetrohydrofuran (THF), has been recently reported.([5,6]) In the latter case, stabilization by THF is claimed to reduce the operation pressure by several orders of magnitude close to room temperature. Here, we apply in situ neutron diffraction to show that-in contrast to previous reports([5,6]) - hydrogen (deuterium) occupies the small cages of the clathrote hydrate only to 30% (at 274 K and 90.5 bar). Such a D-2 load is equivalent to 0.27 wt. % of stored H-2. In addition, we show that a surplus of D2O results in the formation of additional D2O ice Ih instead of in the production of sub-stoichiometric clathrate that is stabilized by loaded hydrogen (as was reported in ref. [6]). Structure-refinement studies show that [D-8]THF is dynamically disordered, while it fills each of the large cages of [D-8]THF center dot 17D(2)O stoichiometrically. Our results show that the clathrate hydrate takes up hydrogen rapidly at pressures between 60 and 90 bar (at about 270 K). At temperatures above approximate to 220 K, the H-storage characteristics of the clathrate hydrate have similarities with those of surface-adsorption materials, such as nanoporous zeolites and metal-organic frameworks,([7,8]) but at lower temperatures, the adsorption rates slow down because of reduced D-2 diffusion between the small cages. © 2008, Wiley-VCH Verlag Berlinen_AU
dc.identifier.citationMulder, F. M., Wagemaker, M., van Eijck, L., & Kearley, G. J. (2008). Hydrogen in porous tetrahydrofuran clathrate hydrate. ChemPhysChem, 9(9), 1331-1337. doi:10.1002/cphc.200700833en_AU
dc.identifier.govdoc1250en_AU
dc.identifier.issn1439-4235en_AU
dc.identifier.issue9en_AU
dc.identifier.journaltitleChemPhysChemen_AU
dc.identifier.pagination1331-1337en_AU
dc.identifier.urihttp://dx.doi.org/10.1002/cphc.200700833en_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/1330en_AU
dc.identifier.volume9en_AU
dc.language.isoenen_AU
dc.publisherWiley-VCH Verlag Berlinen_AU
dc.subjectHydrogenen_AU
dc.subjectTetrahydrofuranen_AU
dc.subjectClathratesen_AU
dc.subjectHydratesen_AU
dc.subjectPorous materialsen_AU
dc.subjectDiffusionen_AU
dc.titleHydrogen in porous tetrahydrofuran clathrate hydrateen_AU
dc.typeJournal Articleen_AU
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