Large-Cage Occupancies of Hydrogen in Binary Clathrate Hydrates Dependent on Pressures and Guest Concentrations

Sugahara, Takeshi; Haag, Joanna C.; Warntjes, Ashleigh A.; Prasad, Pinnelli S. R.; Sloan, E. Dendy; Koh, Carolyn A.; Sum, Amadeu K.

doi:10.1021/jp105379x

Cited by 73 publications

(50 citation statements)

References 32 publications

(115 reference statements)

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“…17 Recent experimental results support the idea that the hydrogen content of promoted clathrates may indeed be tunable, with a reported hydrogen content of around 3.5 wt% in THF/acetone H 2 -H 2 O clathrates. 18,19 However, this number does not yet meet the DOE target.…”

Section: Introductionmentioning

confidence: 99%

A multifaceted approach to hydrogen storage

Churchard

Banach

Borgschulte

et al. 2011

Phys. Chem. Chem. Phys.

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The widespread adoption of hydrogen as an energy carrier could bring significant benefits, but only if a number of currently intractable problems can be overcome. Not the least of these is the problem of storage, particularly when aimed at use onboard light-vehicles. The aim of this overview is to look in depth at a number of areas linked by the recently concluded HYDROGEN research network, representing an intentionally multi-faceted selection with the goal of advancing the field on a number of fronts simultaneously. For the general reader we provide a concise outline of the main approaches to storing hydrogen before moving on to detailed reviews of recent research in the solid chemical storage of hydrogen, and so provide an entry point for the interested reader on these diverse topics. The subjects covered include: the mechanisms of Ti catalysis in alanates; the kinetics of the borohydrides and the resulting limitations; novel transition metal catalysts for use with complex hydrides; less common borohydrides; protic-hydridic stores; metal ammines and novel approaches to nano-confined metal hydrides.

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Section: Introductionmentioning

confidence: 99%

A multifaceted approach to hydrogen storage

Churchard

Banach

Borgschulte

et al. 2011

Phys. Chem. Chem. Phys.

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“…Recently, hydrogen has received a great deal of attention in the hydrate community owing to its high potential for use in energy‐related and many other issues 7. 8 Numerous studies concerning hydrogen storage using clathrate hydrates have been reported with much efforts aimed at increasing storage capacity, introducing unusual tuning effects by changes in concentration and pressure 9–11. Another interesting observation about hydrogen is that atomic hydrogen radicals can be captured stably in the water cages of clathrate hydrates 2.…”

Section: Introductionmentioning

confidence: 99%

Abnormal Thermal Expansion of Clathrate Hydrates Induced by Asymmetric Guest Molecules

Cha¹,

Youn²,

Kwon³

et al. 2011

Chemistry An Asian Journal

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We investigated for the first time the abnormal thermal expansion induced by an asymmetric guest structure using high-resolution neutron powder diffraction. Three dihydrogen molecules (H(2), D(2), and HD) were tested to explore the guest dynamics and thermal behavior of hydrogen-doped clathrate hydrates. We confirmed the restricted spatial distribution and doughnut-like motion of the HD guest in the center of anisotropic sII-S (sII-S=small cages of structure II hydrates). However, we failed to observe a mass-dependent relationship when comparing D(2) with HD. The use of asymmetric guest molecules can significantly contribute to tuning the cage dimension and thus can improve the stable inclusion of small gaseous molecules in confined cages.

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“…With a further increase in pressure, Raman peaks of triple-and quadruple-H 2 clusters were detected at ∼550 and ∼700 bar, respectively. 19 Note that conflicting arguments pertaining to experimental and simulation results have previously been raised regarding double H 2 occupancy in the 5 12 cage. 20−23 Figures 1 and 2 show Raman peaks corresponding to H 2 vibrons in hydrate samples with χ THF and χ PRD values of 0.01, respectively.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Effect of Molecular Nitrogen on Multiple Hydrogen Occupancy in Clathrate Hydrates

et al. 2014

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Multiple H 2 occupancy in confined cages has been explored for the purpose of enhancing storage capacity. Furthermore, balancing the formation pressure with high storage capacity is one of the most significant factors. Here, we demonstrate the use of binary (LGM + N 2 ) hydrates to capture hydrogen clusters under relatively mild conditions, even observing double H 2 occupancy in small cages. The cage occupancy and structures of hydrates were identified by the Raman spectroscopic analysis and highresolution powder diffraction. The reaction product of binary (LGM + N 2 ) hydrates with H 2 molecules suggests the possibility of multiple H 2 occupancy in both small (5 12 ) and large (5 12 6 4 ) cages at relatively low pressures. Also, the lattice parameter decreases with an increase in H 2 occupancy. The unique and abnormal role of N 2 as a preoccupied coguest significantly affects the H 2 population in a crystalline hydrate matrix and further lowers the pressure for structure stabilization.

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Large-Cage Occupancies of Hydrogen in Binary Clathrate Hydrates Dependent on Pressures and Guest Concentrations

Cited by 73 publications

References 32 publications

A multifaceted approach to hydrogen storage

A multifaceted approach to hydrogen storage

Abnormal Thermal Expansion of Clathrate Hydrates Induced by Asymmetric Guest Molecules

Effect of Molecular Nitrogen on Multiple Hydrogen Occupancy in Clathrate Hydrates

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