Nickel(II) complex was utilized as a sustainable catalyst for α-alkylation of arylacetonitriles with challenging secondary alcohols. Arylacetonitriles with a wide range of functional groups were tolerated, and various cyclic and acyclic secondary alcohols were utilized to yield a large number of α-alkylated products. The plausible mechanism involves the base-promoted activation of precatalyst to an active catalyst (dehydrochlorinated product) which activates the O-H and C-H bonds of the secondary alcohol in a dehydrogenative pathway.
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