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Singly NHC‐coordinated (aminoboryl)aminoborenium salts react with Na2[Fe(CO)4] to yield stable coordination complexes of aminoborylene‐stabilized aminoborylenes, which exhibit exceptional σ‐donor properties. Upon photolytic CO extrusion from the metal center, the diboron ligand adopts a novel η3‐BBN coordination mode, where bond‐strengthening backdonation from the metal center into the vacant B−B...
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