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Metal borohydrides are a fascinating and continuously expanding class of materials, showing promising applications within many different fields of research. This study presents 17 derivatives of the hydrogen-rich ammonium borohydride, NH4BH4, which all exhibit high gravimetric hydrogen densities (9.2 wt % of H2). A detailed insight into the crystal structures combining X-ray diffraction and density functional theory calculations exposes an intriguing structural variety ranging from three-dimensional (3D) frameworks, 2D-layered, and 1
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