Abstract
Mixed alkali alanates LixNa3-xAlH6 have been successfully synthesized by means of grinding mixtures of Li3AlH6 and Na3AlH6 in specific molar ratios. Non-stoichiometric LixNa3-xAlH6 compounds with single perovskite-type structures (space group Fm-3m) can be formed only within the composition range of x = 0.9–1.3. Li1.3Na1.7AlH6 exhibits superior hydrogen storage properties over other LixNa3-xAlH6 compounds. Its onset dehydrogenation temperature (∼423 K) was lowered by more than 40 K from other samples in temperature programmed dehydrogenation (TPD) curves. Also, the dehydrogenation capacity of Li1.3Na1.7AlH6 (3.45 wt.%) is the highest among the compounds. The dehydrogenation enthalpy values of LixNa3-xAlH6 decreased as x increased from 0.9 to 1.3 according to the results by isothermal pressure-composition (PCI) curves and van't Hoff plots. It shows that the dehydrogenation Li1.3Na1.7AlH6 (49.7 kJ mol H2−1) was greatly destabilized from that of LiNa2AlH6 (68.1 kJ mol H2−1). Furthermore, the apparent activation energy of dehydrogenation for Li1.3Na1.7AlH6 (138.1 kJ mol−1) was remarkably lowered from that of LiNa2AlH6. This illustrates that Li1.3Na1.7AlH6 exhibits enhanced dehydrogenation kinetics from that of LiNa2AlH6.
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