Lithium aluminum hydride (LiAlH4) is a promising compound for hydrogen storage, with a high gravimetric and volumetric hydrogen density and a low decomposition temperature. Similar to other metastable hydrides, LiAlH4 does not form by direct hydrogenation at reasonable hydrogen pressures; therefore, there is considerable interest in developing new routes to regenerate the material from the dehydrogenated products LiH and Al. Here we demonstrate a low-energy route to regenerate LiAlH4 from LiH and. Ti-catalyzed Al. The initial hydrogenation occurs in a tetrahydrofuran slurry and forms the adduct LiAlH4 center dot 4THF. The thermodynamics of this reversible reaction were investigated by measuring pressure-composition isotherms, and the free energy was found to be small and slightly negative (Delta G = -1.1 kJ/mol H-2) suggesting an equilibrium hydrogen pressure of just under 1 bar at 300 K. We also demonstrate that the adduct LiAlH4 center dot 4THF can be desolvated at low temperature to yield crystalline LiAlH4.