α‐Alkylation of Ketones Using Benzylic Alcohols Catalyzed by [(η⁶‐p‐cymene)RuLCl][PF₆] {L = Di(pyridin‐2‐yl)amine}

A cationic complex, [(η 6 ‐p‐cymene)RuLCl] + [PF 6 ] − (1) {L = di(pyridin‐2‐yl)amine}, has been synthesized from the reaction of [(η 6 ‐p‐cymene)RuCl 2 ] 2 with di(pyridin‐2‐yl)amine in acetonitrile. The complex has been characterized by 1 H and 13 C nuclear magnetic resonance spectroscopy and high‐resolution mass spectrometry. Additionally, the complex has been structurally characterized. This complex has been used as a homogeneous catalyst for the α‐alkylation of ketones with benzylic alcohols as an alkylating agent in toluene at 120 °C in the presence of Cs 2 CO 3 . The scope of the reaction extends to the synthesis of a fluorescent α‐alkylated product. Mechanistic insights suggest that the water molecule generated in situ during the aldol condensation facilitates the reactivation of the catalytic species, thereby sustaining the catalytic cycle.