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.