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Application of the diamide, diimine {-CH[double bond, length as m-dash]N(1,2-C 6 H 4 )N(2,6- i Pr 2 -C 6 H 3 )} 2   m  ((dadi)  m  ) ligand to titanium provided adducts (dadi)TiL  x  ( 1 -L  x  ; L  x  = THF, PMe 2 Ph, (CNMe) 2 ), which possess the redox formulation [(dadi) 4- ]Ti(iv)L  x  , and 22 πe - (4 n + 2). Related complexes containing titanium-ligand multiple bonds, (dadi)Ti[double bond, length as m-dash]X ( 2 [double bond, length as m-dash]X; X = O, NAd), exhibit a different dadi redox state, [(dadi) 2- ]Ti(iv)X, consistent with 20 πe - (4 n ). The Redox Non-Innocence (RNI) displayed by dadi  m  impedes binding by CO, and permits catalytic conversion of AdN 3 + CO to AdNCO + N 2 . Kinetics measurements support carbonylation of 2 [double bond, length as m-dash]NAd as the rate determining step. Structural and computational evidence for the observed RNI is provided.

Redox non-innocence permits catalytic nitrene carbonylation by (dadi)TiNAd (Ad = adamantyl)