Alloying with Si is shown to destabilize the strongly bound hydrides LiH and MgH2. For the LiH/Si system, a Li2.35Si alloy forms upon dehydrogenation, causing the equilibrium hydrogen pressure at 490 degreesC to increase from approximately 5 x 10(-5) to 1 bar. For the MgH2/Si system, Mg2Si forms upon dehydrogenation, causing the equilibrium pressure at 300 degreesC to increase from 1.8 to > 7.5 bar. Thermodynamic calculations indicate equilibrium pressures of 1 bar at approximately 20 degreesC and 100 bar at approximately 150 degreesC. These conditions indicate that the MgH2/Si system, which has a hydrogen capacity of 5.0 wt %, could be practical for hydrogen storage at reduced temperatures. The LiH/Si system is reversible and can be cycled without degradation. Absorption/desorption isotherms, obtained at 400-500 degreesC, exhibited two distinct flat plateaus with little hysteresis. The plateaus correspond to formation and decomposition of various Li silicides. The MgH2/Si system was not readily reversible. Hydrogenation of Mg2Si appears to be kinetically limited because of the relatively low temperature, < 150 degreesC, required for hydrogenation at 100 bar. These two alloy systems show how hydride destabilization through alloy formation upon dehydrogenation can be used to design and control equilibrium pressures of strongly bound hydrides.