Polymer‐Anchored Bifunctional Pincer Catalysts for Chemoselective Transfer Hydrogenation and Related Reactions

A series of polymer‐supported cooperative PC(sp3)P pincer catalysts was synthesized and characterized. Their catalytic activity in the acceptorless dehydrogenative coupling of alcohols and the transfer hydrogenation of aldehydes with formic acid as a hydrogen source was investigated. This comparative study, examining homogeneous and polymer‐tethered species, proved that carefully designing a link between the support and the catalytic moiety, which takes into consideration the mechanism underlying the target transformation, might lead to superior heterogeneous catalysis. Just a pinch: Efficient, recoverable, and durable polymer‐supported bifunctional cooperative PC(sp3)P pincer catalysts are described for use in acceptorless dehydrogenative coupling of alcohols and transfer hydrogenation of aldehydes, highlighting that carefully designing a link between the support and the catalytic moiety may lead to superior heterogeneous catalysis.