Abstract
In the search for hydrogen-storage materials with a high gravimetric capacity, Mg(y)Ti((1-y)) alloys, which exhibit excellent kinetic properties, form the basis for more advanced compounds. The plateau pressure of the Mg--Ti--H system is very low (approximately 10(-6) bar at room temperature). A way to increase this pressure is by destabilizing the metal hydride. The foremost effect of incorporating an additional element in the binary Mg--Ti system is, therefore, to decrease the stability of the metal hydride. A model to calculate the effect on the thermodynamic stability of alloying metals was developed by Miedema and co-workers. Adopting this model offers the possibility to select promising elements beforehand. Thin films consisting of Mg and Ti with Al or Si were prepared by means of e-beam deposition. The electrochemical galvanostatic intermittent titration technique was used to obtain pressure-composition isotherms for these ternary materials and these isotherms reveal a reversible hydrogen-storage capacity of more than 6 wt. %. In line with the calculations, substitution of Mg and Ti by Al or Si indeed shifts the plateau pressure of a significant part of the isotherms to higher pressures, while remaining at room temperature. It has been proven that, by controlling the chemistry of the metal alloy, the thermodynamic properties of Mg-based hydrides can be regulated over a wide range. Hence, the possibility to increase the partial hydrogen pressure, while maintaining a high gravimetric capacity creates promising opportunities in the field of hydrogen-storage materials, which are essential for the future of the hydrogen economy.
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