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New iron complexes [Cp*Fe L ] −  ( 1‐σ and 1‐π , Cp*=C 5 Me 5 ) containing the chelating phosphinine ligand 2‐(2′‐pyridyl)‐4,6‐diphenylphosphinine ( L ) have been prepared, and found to undergo facile reaction with CO 2  under ambient conditions. The outcome of this reaction depends on the coordination mode of the versatile ligand  L . Interaction of CO 2  with the isomer  1‐π , in which  L  binds to Fe through the phosphinine moiety in an η 5  fashion, leads to the formation of  3‐π , in which CO 2  has undergone electrophilic addition to the phosphinine group. In contrast, interaction with  1‐σ —in which  L  acts as a σ‐chelating [P,N] ligand—leads to product  3‐σ  in which one C=O bond has been completely broken. Such CO 2  cleavage reactions are extremely rare for late 3d metals, and this represents the first such example mediated by a single Fe centre.

Facile C=O Bond Splitting of Carbon Dioxide Induced by Metal–Ligand Cooperativity in a Phosphinine Iron(0) Complex