Complex hydrides represent potential materials with high hydrogen capacity and practical thermodynamics, which makes them favorable candidates for hydrogen storage for transportation applications. Although our early work has shown that these materials are promising, additional improvement in their characteristics was required. The aim of this research is to further improve the kinetics of complex hydrides alanate materials and to advance their suitability for hydrogen storage by modifying their composition and morphology. In order to achieve these objectives novel methods were developed to alter and form complex hydride compounds with desired characteristics. Thermodynamic study, kinetic measurements, X-ray analysis and spectroscopic investigation are reported. The experimental effort was guided by theoretical modeling.