A new ternary complex hydride is synthesized by the interaction between LiNH and LiBH. The crystal structure of this new hydride is tentatively indexed using an orthorhombic cell with a space group of 2 and lattice parameters of = 9.643 Å, = 6.228 Å, and = 5.563 Å. The LiNH-2LiBH sample shows excellent hydrogenation properties with hydrogen absorption starting at near-ambient temperature (50 °C), which is more than 100 °C lower than that of pristine LiNH. Furthermore, it attains 100% hydrogenation under isothermal conditions at 60 °C and 50 bar hydrogen pressure. Such superior low-temperature hydrogen absorption may be due to the formation of this new complex hydride. Interestingly, above 97 °C, the lithium-ion conductivity of this new hydride is higher than those of LiNH and LiBH and reaches 10 S cm at 114 °C. Meanwhile, the ionic conductivity of this new hydride is ∼30 times higher than that of LiBH reaching 10 S cm at room temperature. The interaction between imides and borohydrides described in this work expands the options for strategic design of novel hydrogen storage materials and solid ionic conductors.
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