Integrated "all-in-one" strategy to construct highly efficient Pd catalyst for CO transformation.

The synthesis of high-value chemicals featuring C-C and/or C-heteroatom bonds CO is critically important, yet efficiently converting thermodynamically stable and kinetically inert linear CO and propargylic amine to the heterocyclic compound 2-oxazolidinone with an integrated catalytic system continues to pose a considerable challenge. Herein, we have designed an "all-in-one" (AIO) palladium (Pd) catalyst (Cat1), distinguished by its co-coordination with acetylglucose (AcGlu) and bis(benzimidazolium) units at the Pd center, which promotes the cyclization of CO and propargylic amine achieving a highest turnover frequency (TOF) of up to 3456 h. Moreover, Cat1 demonstrates excellent stability across various temperatures, with its catalytic activity remaining unchanged even after 10 cycles. The catalyst Cat1 simultaneously activates propargylic amine and CO, facilitating the formation of N-heterocyclic carbene (NHC)-CO adducts and AcGlu-CO philes from CO in simulated flue gas, a key factor in reaching unprecedented TOF values. The catalytic mechanism was elucidated through NMR and C-isotope labeling experiments. Notably, this is the first instance of an AIO Pd catalyst that enables the simultaneous capture, activation, and catalytic conversion of activated CO along with propargylic amine. The design strategy of this AIO catalyst introduces a novel approach to overcoming the challenges in the efficient conversion of inert CO.