Abstract
Lithium borohydride, LiBH(4), possesses high hydrogen capacity, but cannot be used for hydrogen storage owing to the problematic H-exchange kinetics and thermodynamics. In the present study, we employed the Li(+)-Ca(2+) combination strategy to improve the de/rehydrogenation properties of LiBH4. Our study found that mechanically milling 1:1 LiBH(4)/Ca(BH(4))(2) mixture formed a dual-cation borohydride, Li(0.9)Ca(BH(4))(2.9), which then transformed to stoichiometric LiCa(BH(4))(3) in the heating process. The formation and decomposition behaviors of LiCa(BH(4))(3) were studied using X-ray diffraction and thermogravimetry/differential scanning calorimetry/mass spectroscopy techniques. It was found that LiCa(BH(4))(3) differs significantly from the component phases in terms of physical properties, decomposition behaviors, and mechanistic pathway. In particular, LiCa(BH(4))(3) exhibits improved de/rehydrogenation properties relative to the component phases. These experimental findings exemplified the effectiveness of manipulation of dual-cation combination in tuning the de/rehydrogenation properties of the ionic light-metal borohydrides.
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