2‑Pyridonate Tantalum Complexes for the Intermolecular Hydroaminoalkylation of Sterically Demanding Alkene​s

The design and synthesis of a mixed 2-pyridonate-Ta­(NMe2)3Cl complex for the direct C–H alkylation adjacent to nitrogen in unprotected secondary amines are reported. The hydro­amino­alkyl­ation of sterically demanding internal alkenes gives the direct, catalytic formation of C­(sp3)–C­(sp3) bonds. Substrate scope investigations reveal key strategies for further catalyst development efforts in this 100% atom-economic synthesis of α-alkylated amines.