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Molecular Hydrogen Storage in Binary THF−H 2 Clathrate Hydrates

2006; American Chemical Society; Volume: 110; Issue: 34 Linguagem: Inglês

10.1021/jp062139n

1520-6106

Timothy A. Strobel, Craig J. Taylor, Keith C. Hester, Steven F. Dec, Carolyn A. Koh, Kelly T. Miller, E. Dendy Sloan,

Spacecraft and Cryogenic Technologies

The hydrogen storage capacity of binary THF−H2 clathrate hydrate has been determined as a function of formation pressure, THF composition, and time. The amount of hydrogen stored in the stoichiometric hydrate increases with pressure and exhibits asymptotic (Langmuir) behavior to approximately 1.0 wt % H2. This hydrogen concentration corresponds to one hydrogen molecule occupying each of the small 512 cavities and one THF molecule in each large 51264 cavity in the hydrate framework. Contrary to previous reports, hydrogen storage was not increased upon decreasing the THF concentration below the stoichiometric 5.6 mol % solution to 0.5 mol %, at constant pressure, even after one week. This provides strong evidence that THF preferentially occupies the large 51264 cavity over hydrogen, for the range of experimental conditions tested. The maximum amount of hydrogen stored in this binary hydrate was about 1.0 wt % at moderate pressure (<60 MPa) and is independent of the initial THF concentration over the range of conditions tested.