We tune the thermodynamics of hydrogen absorption in Mg by means of elastic clamping. The loading isotherms measured by hydrogenography show that Mg films covered with Mg-alloy-forming elements, such as Pd and Ni, have hydrogen plateau pressures more than 2 orders of magnitude higher than bulk Mg at the same temperature. An elastic model allows us to interpret the Mg thickness dependence of the hydrogen plateau pressure. Our results suggest an alternative route for the development of new hydrogen storage materials with optimized thermodynamic properties.

A detailed structural analysis of Mg-Ti-H thin films reveals the presence of a chemically partially segregated but structurally coherent metastable phase. By combining X-Ray Diffraction and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy on Mg_yTi_1-yH_x thin films we find non-zero Chemical Short-Range Order (CSRO) parameters for all the compositions measured. Despite the positive enthalpy of mixing of Mg and Ti the degree of ordering does not increase upon loading and unloading with hydrogen. The robustness of this system and the fast and reversible kinetics of hydrogen loading and unloading are caused by the formation of nanoscale compositional modulations in the intermetallic alloy. This microstructure is responsible for the exceptional properties of Mg_yTi_1-yH_x thin films. It also shows that reversible metastable metal-hydrides offer new possibilities for hydrogen storage, beyond the limits imposed by thermodynamic equilibrium.

The reflection and transmission spectra of Pd capped Mg_y Ti_{1 - y} thin films (y = 0.7, 0.8 and 0.9) are measured in the 0.5-5.5 eV energy range, both in the as-prepared and hydrogenated states. Upon hydrogenation these films switch reversibly from a shiny metallic state into a "black" absorbing one. The composition and thicknesses can be tailored to achieve high solar absorptance and low thermal emittance in the hydrogenated state. The combination of these two characteristics is interesting for the application of this material as switchable absorber in solar collectors. The use of a Mg_y Ti_{1 - y} switchable absorber in solar collectors allows to lower the stagnation temperature from 180 to 80 °C. The collector efficiency is affected only minimally.

The structural, optical, and electrical transformations induced by hydrogen absorption and/or desorption in Mg-Ti thin films prepared by co-sputtering of Mg and Ti are investigated. Highly reflective in the metallic state, the films become highly absorbing upon H absorption. The reflector-to-absorber transition is fast, robust, and reversible over many cycles. Such a highly absorbing state hints at the coexistence of a metallic and a semiconducting phase. It is, however, not simply a composite material consisting of independent Mg H2 and Ti H2 grains. By continuously monitoring the structure during H uptake, we obtain data that are compatible with a coherent structure. The average structure resembles rutile Mg H2 at high Mg content and is fluorite otherwise. Of crucial importance in preserving the reversibility and the coherence of the system upon hydrogen cycling is the accidental equality of the molar volume of Mg and Ti H2. The present results point toward a rich and unexpected chemistry of Mg-Ti-H compounds.

Mg-Ti-H thin films are found to have very attractive optical properties: they absorb 87% of the solar radiation in the hydrogenated state and only 32% in the metallic state. Furthermore, in the absorbing state Mg-Ti-H has a low emissivity; at 400 K only 10% of blackbody radiation is emitted. The transition between both optical states is fast, robust, and reversible. The sum of these properties highlights the applicability of such materials as switchable smart coatings in solar collectors.