We propose a reversible hydrogen storage mechanism for cycled sodium alanate. The individual mechanistic reaction steps for the decomposition reaction derive a set of time-dependent differential equations that simultaneously produce the evolution plots for each species. These plots reproduce several aspects of in situ X-ray diffraction (XRD) data, as well as the measured relative composition of selected decomposition samples at various extents of reaction. The presence of alanes facilitates both the decomposition and reformation of sodium alanate based on the principle of microscopic reversibility. A major role for the titanium dopant in catalyzed sodium alanate dynamics may be alloy formation at or near the surface of bulk aluminum that facilitates the formation and sorption properties of alanes. Published by Elsevier B.V.