While uranium hydridoborate complexes
containing the [BH<sub>4</sub>]<sup>−</sup> moiety have been
well-known in the literature for many years, species with functionalized
borate centers remained considerably rare. We were now able to prepare
several uranium hydridoborates (<b>1–4</b>) with amino-substituted
borate moieties with high selectivity by smooth reaction of [Cp*<sub>2</sub>UMe<sub>2</sub>] (Cp* = C<sub>5</sub>Me<sub>5</sub>) and [Cp′<sub>2</sub>UMe<sub>2</sub>] (Cp′ = 1,2,4-<i>t</i>Bu<sub>3</sub>C<sub>5</sub>H<sub>2</sub>) with the aminoborane H<sub>2</sub>BN(SiMe<sub>3</sub>)<sub>2</sub>. A combination of nuclear magnetic
resonance spectroscopy, deuteration experiments, magnetic SQUID measurements,
and X-ray/neutron diffraction studies was used to verify the anticipated
molecular structures and oxidation states of <b>1–4</b> and helped to establish a linear tridentate coordination mode of
the borate anions