We have prepared the transition metal borohydride hydrazinates (ZBH) for the first time. Zn(BH4)2-2N2H4 exhibits pure hydrogen evolution below 200 °C as determined by thermogravimetric-differential thermal analysis (TG-DTA) coupled with mass spectroscopy (MS). We now wish to investigate the mechanisms of ZBH formation and dehydrogenation via in-situ powder neutron diffraction (PND) technique. By employing in-situ neutron diffraction technique we will be able to determine the structures of intermediates regarding ZBH formation and dehydrogenation process. Moreover, PND can help to elucidate the coordination chemistry of N2H4 (N2D4) and [BH4]- ([BD4]-) moieties relative to the metal center in the intermediate phases and be crucial to verify the [BD4]- and possibly N2D4 dynamic disorder by precisely locating the positions of H (D), Li, 11B, and N which are not reasonably diffracted by XRD.