Tetranuclear cores (M-E) of transition metals (M) and tetrylenes (E=Si, Ge, Sn) are key motifs in homogeneous and heterogeneous catalysis. They exhibit a continuum of M-M and E-E bonding within the inorganic core that leads to a variety of structures for which there are no specific synthetic methods. Herein, we report a series of highly reduced [NiGe] squares solely stabilized by bulky terphenyl (CH-2,6-Ar) ligands, for which we provide complementary and high-yielding syntheses. Reactivity studies with common Lewis bases (carbene and CO) evince that the structure of the (M-E) core can be transformed. We have investigated this core modification by computational means, offering a rationale to better understand the continuum of bonding across these clusters.
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