Reversible Redox Ligand-Centered Reactivity in 2,6-Bisiminopyridine Aluminum Systems

We report the synthesis of cationic 2,6-bisiminopyridine organoaluminum complexes, [(BIP)AlR₂]⁺, as stable BAr^F₄^- or PF₆^- salts, and their reversible single-electron reduction into well-defined paramagnetic species, [(BIP·)AlR₂]. Four redox couples, [(BIP)AlR₂]^+/0, have been fully characterized through structural, spectroscopic, electrochemical and computational techniques.