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• W2247161069 abstract "The project was component of the US DOE, Metal Hydride Center of Excellence (MHCoE). The Sandia National Laboratory led center was established to conduct highly collaborative and multi-disciplinary applied RD screening of catalysts for high capacity materials requiring kinetics enhancement; development of low temperature methods for nano-confinement of hydrides and determining its effects on the kinetics and thermodynamics of hydrides; and development of novel processes for the direct re-hydrogenation of materials. These efforts have resulted in several advancements the development of hydrogen storage materials. We have greatly extended the fundamental knowledge about the highly promising hydrogen storage carrier, alane (AlH₃), by carrying out the first crystal structure determinations and the first determination of the heats of dehydrogenation of β–AlH₃ and γ-AlD₃. A low-temperature homogenous organometallic approach to incorporation of Al and Mg based hydrides into carbon aerogels has been developed that that allows high loadings without degradation of the nano-porous scaffold. Nano-confinement was found to significantly improve the dehydrogenationmore » kinetics but not effect the enthalpy of dehydrogenation. We conceived, characterized, and synthesized a novel class of potential hydrogen storage materials, bimetallic borohydrides. These novel compounds were found to have many favorable properties including release of significant amounts of hydrogen at moderate temperatures (75-190oC). However, in situ IR studies in tandem with thermal gravimetric analysis have shown that about 0.5 equivalents of diborane are released during the dehydrogenation making re-hydrogenation effectively impossible and precluding these compounds from further consideration as hydrogen storage materials. The hydrogen cycling of >11 wt % between MgB₂ to Mg(BH₄)₂ was achieved but required very forcing conditions. Under moderate conditions (dehydrogenation 200°C; re-hydrogenation 250°C, 120 atm H2), Mg(BH₄)₂ undergoes reversible dehydrogenation to Mg(B3H8)2. Although the 2.5 wt% cycling capacity does not meet current on-board storage targets, this result provides first example of direct hydrogen cycling of a borohydride under moderate conditions and demonstrates the plausibility of finding mild, PEM fuel cell relevant conditions for the high capacity, reversible dehydrogenation of borohydrides. A method was developed for the room temperature, direct hydrogenation of Ti-doped LiH/Al in liquefied dimethyl ether under 100 atm of H₂. The process has been optimized such that Ti-doped LiAlH₄ is obtained in >95% yield. The WTT energy efficiency our direct synthesis process has been estimated to approach the 60% U.S. DOE target. Thus our simplification of the hydrogenation half-cycle may provide the key to harnessing the long-recognized potential of this lightweight, high capacity material as a practical hydrogen carrier. Finally, we have gained insight into the fundamental basis of the enhanced hydrogen cycling kinetics of Ti-doped NaAlH₄ through studies by solid state ¹H NMR, anelastic spectroscopy; muon spin rotation; and positron annihilation.« less" @default.
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• W2247161069 date "2013-05-31" @default.
• W2247161069 modified "2023-10-16" @default.
• W2247161069 title "Final Report: DE- FC36-05GO15063, Fundamental Studies of Advanced High-Capacity, Reversible Metal Hydrides" @default.
• W2247161069 doi "https://doi.org/10.2172/1169445" @default.
• W2247161069 hasPublicationYear "2013" @default.
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