The exceptional reactivity of the decamethylsamarocene–THF adduct Cp 2*Sm(thf)2 is revealed in the reaction with tBuC P, which results in reductive dimerization of the phosphaalkyne and formation of the dinuclear complex 1 in 40% yield. Complex 1 contains the dinion of 2,3‐diphosphabutadiene as a novel ligand.
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