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The versatile coordination behavior of the P 4  butterfly complex [{Cp*Cr(CO) 3 } 2 (μ,η 1:1 ‐P 4 )] ( 1 ) towards Lewis acidic pentacarbonyl compounds of Cr, Mo and W is reported. The reaction of  1  with [W(CO) 4 (nbd)] (nbd=norbornadiene) yields the complex [{Cp*Cr(CO) 3 } 2 (μ 3 ,η 1:1:1:1 ‐P 4 ){W(CO) 4 }] ( 2 ) in which  1  serves as a chelating P 4  butterfly ligand. In contrast, reactions of  1  with [M(CO) 4 (nbd)] (M=Cr ( a ), Mo ( b )) result in the step‐wise formation of [{Cp*Cr(CO) 2 } 2 (μ 3 ,η 3:1:1 ‐P 4 ){M(CO) 5 }] ( 3 a,b ) and [{Cp*Cr(CO) 2 } 2 ‐(μ 4 ,η 3:1:1:1 ‐P 4 ){M(CO) 5 } 2 ] ( 4 a,b ) which contain a folded cyclo‐P 4  unit. Complex  4 a  undergoes an unprecedented P 1 /P 3 ‐fragmentation yielding the cyclo‐P 3  complex [Cp*Cr(CO) 2 (η 3 ‐P 3 )] ( 5 ) and the as yet unknown phosphinidene complex [Cp*Cr(CO) 2 {Cr(CO) 5 } 2 (μ 3 ‐P)] ( 6 ). The identity of  6  is confirmed by spectroscopic methods and by the in situ formation of [{Cp*Cr(CO) 2 ( t BuNC)}P{Cr(CO) 5 } 2 ( t BuNC)] ( 7 ). DFT calculations throw light on the bonding situation of the reported products.

The Butterfly Complex [{Cp*Cr(CO) 3 } 2 (μ,η 1:1 ‐P 4 )] as a Versatile Ligand and Its Unexpected P 1 /P 3 Fragmentation