Catalytic alkane dehydrogenation is a reaction with tremendous potential for application. We describe a highly active PSCOP‐pincer iridium catalyst for transfer dehydrogenation of cyclic and linear alkanes. The dehydrogenation of linear alkanes occurs under relatively mild conditions with high regioselectivity for α‐olefin formation. In addition, the catalyst system is very effective in the dehydrogenation of heterocycles to form heteroarenes and olefinic products.

A series of new hydrido Ru­(II) olefin complexes supported by isopropyl-substituted pincer ligands have been synthesized and characterized. These complexes are thermally robust and active for catalytic transfer and acceptorless alkane dehydrogenation. Notably, the alkane dehydrogenation catalysts are tolerant of a number of polar functional species.

The first α-alkylation of unactivated amides with primary alcohols is described. An effective and robust iridium pincer complex has been developed for selective α-alkylation of tertiary and secondary acetamides involving a "borrowing hydrogen" methodology. The method is compatible with alcohols bearing various functional groups. This presents a convenient and environmentally benign protocol for α-alkylation of amides.

The selective catalytic reduction of amides to value-added amine products is a desirable but challenging transformation. Pharmaceutical agents and fluorescent materials routinely contain amine motifs. Here we present a combined...