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• W4323822260 endingPage "6111" @default.
• W4323822260 startingPage "6100" @default.
• W4323822260 abstract "Privileged diphosphine ligands that chelate many transition metals to form stable chelation complexes are essential in a variety of catalytic processes. However, the exact identity of the catalytically active moieties remains ambiguous because the chelated metal catalysts may undergo rearrangement during catalysis to produce monophosphine-metal complexes, which are hard to isolate and evaluate the activities. By taking advantage of the isolation of two phosphorus atoms, we demonstrate here the successful construction of chiral monophosphine-Ir/Ru complexes of diphosphine ligands in covalent organic frameworks (COFs) for enantioselective hydrogenation. By condensation of the tetraaldehyde of enantiopure MeO-BIPHEP and linear aromatic diamines, we prepare two homochiral two-dimensional COFs with ABC stacking, in which the two P atoms of each diphosphine are separated and fixed far apart. Post-synthetic metalations of the COFs thus afford the single-site Ir/Ru-monophosphine catalysts, in contrast to the homogeneous chelated analogues, that demonstrated excellent catalytic and recyclable performance in the asymmetric hydrogenation of quinolines and β-ketoesters, affording up to 99.9% enantiomeric excess. Owing to the fact that the porous catalyst is capable of adsorbing and concentrating hydrogen, the catalytic reactions are promoted under ambient/medium pressure, which are typically performed under high pressure for homogeneous catalysis. This work not only shows that monophosphine-metal complexes of diphosphines can be catalytically active centers for asymmetric hydrogenation reactions but also provides a new strategy to prepare new types of privileged phosphine-based heterogeneous catalysts." @default.
• W4323822260 created "2023-03-11" @default.
• W4323822260 creator A5006296753 @default.
• W4323822260 creator A5007046740 @default.
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• W4323822260 creator A5025618145 @default.
• W4323822260 creator A5036930387 @default.
• W4323822260 creator A5040070851 @default.
• W4323822260 date "2023-03-10" @default.
• W4323822260 modified "2023-10-16" @default.
• W4323822260 title "Construction of Monophosphine–Metal Complexes in Privileged Diphosphine-Based Covalent Organic Frameworks for Catalytic Asymmetric Hydrogenation" @default.
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