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- W4280495598 abstract "Abstract Ultrathin two‐dimensional metal–organic framework nanosheets have emerged as a promising kind of heterogeneous catalysts. Herein, we report a series of 2D porphyrinic metal–organic framework nanosheets (X‐PMOF, X=F, Cl, Br), which was prepared from the self‐assembly of a halogen‐based porphyrin ligand X‐TCPP (X‐TCPP=5‐(4‐halogenatedphenyl)‐10,15,20‐tris(4‐carboxyphenyl)‐porphyrin) and ZrCl 4 in the presence of trifluoroacetic acid as the modulating reagent. The framework of X‐PMOF possessed the ftw topology as in MOF‐525. The lamellar X‐PMOF nanosheets with the thickness of down to 4.5 nm were assembled and aggregated into a flower‐like morphology. With the introduction of iridium(III) atoms into the porphyrin rings, the resultant X‐PMOF(Ir) nanosheets were prepared by a similar method. Catalytic results show that Br‐PMOF(Ir) nanosheets were efficient for CO 2 reduction and aminolysis, giving rise to formamides in high yields under room temperature and atmospheric pressure, and can be recycled and reused for 3 runs. The total turnover number of Br‐PMOF(Ir) after 3 runs was 1644 based on Ir. Mechanistic studies disclose that the high efficiency of Br‐PMOF(Ir) nanosheets was ascribed to three factors, including the superior activation capability of iridium(III) porphyrin for Si−H bonds, more active sites on the external surfaces of Br‐PMOF(Ir) nanosheets, and the defects caused by unsymmetrical porphyrin ligand that increased the framework's affinity towards CO 2 ." @default.
- W4280495598 created "2022-05-22" @default.
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- W4280495598 date "2022-06-10" @default.
- W4280495598 modified "2023-10-14" @default.
- W4280495598 title "Ultrathin Two‐Dimensional Metal–Organic Framework Nanosheets Based on a Halogen‐Substituted Porphyrin Ligand: Synthesis and Catalytic Application in CO<sub>2</sub> Reductive Amination" @default.
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- W4280495598 doi "https://doi.org/10.1002/chem.202200555" @default.
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