We analyzed the elevated temperature volumetric hydrogen sorption behavior of magnesium thin films catalyzed by nano-scale bi-layers of Pd/Ta, Pd/Nb, Pd/Ti and Pd/Fe. Sorption of magnesium catalyzed by pure Pd was determined as a baseline. Sorption cycling demonstrated that when utilizing pure Pd and the Pd/Fe bi-layer catalysts the sorption kinetics of the Mg films rapidly degraded. However with the Pd/Nb, Pd/Ti and Pd/Ta bi-layer catalysts the composite remained cycleable. After multiple sorption cycles the Pd/Nb and Pd/Ti catalyst combinations possessed the fastest kinetics. X-ray diffraction analysis showed that NbH(0.5) and TiH(2) are formed during testing. Basic thermodynamic analysis indicates that NbH(0.5) and TiH(2) should be stable both during absorption and during desorption. We believe that this is why Nb and Ti are the most effective intermediate layers: The elements form stable hydrides at the Mg surfaces preventing complete Pd-Mg interdiffusion and/or acting as hydrogen catalysts and pumps. (C) 2009 Professor T. Nejat veziroglu. Published by Elsevier Ltd. All rights reserved.