Covalent organic frameworks (COFs) are crystalline porous solids with well-defined two- or three-dimensional molecular structures. Although the structural regularity provides this new type of porous material with high potentials in catalysis, no example has been presented so far. Herein, we report the first application of a new COF material, COF-LZU1, for highly efficient catalysis. The easily prepared imine-linked COF-LZU1 possesses a two-dimensional eclipsed layered-sheet structure, making its incorporation with metal ions feasible. Via a simple post-treatment, a Pd(II)-containing COF, Pd/COF-LZU1, was accordingly synthesized, which showed excellent catalytic activity in catalyzing the Suzuki-Miyaura coupling reaction. The superior utility of Pd/COF-LZU1 in catalysis was elucidated by the broad scope of the reactants and the excellent yields (96-98%) of the reaction products, together with the high stability and easy recyclability of the catalyst. We expect that our approach will further boost research on designing and employing functional COF materials for catalysis.
This review summarizes the use of metal-organic frameworks (MOFs) as a versatile supramolecular platform to develop heterogeneous catalysts for a variety of organic reactions, especially for liquid-phase reactions. Following a background introduction about catalytic relevance to various metal-organic materials, crystal engineering of MOFs, characterization and evaluation methods of MOF catalysis, we categorize catalytic MOFs based on the types of active sites, including coordinatively unsaturated metal sites (CUMs), metalloligands, functional organic sites (FOS), as well as metal nanoparticles (MNPs) embedded in the cavities. Throughout the review, we emphasize the incidental or deliberate formation of active sites, the stability, heterogeneity and shape/size selectivity for MOF catalysis. Finally, we briefly introduce their relevance into photo- and biomimetic catalysis, and compare MOFs with other typical porous solids such as zeolites and mesoporous silica with regard to their different attributes, and provide our view on future trends and developments in MOF-based catalysis.
Halide perovskite quantum dots (QDs), primarily regarded as optoelectronic materials for LED and photovoltaic devices, have not been applied for photochemical conversion (e.g., water splitting or CO reduction) applications because of their insufficient stability in the presence of moisture or polar solvents. Herein, we report the use of CsPbBr QDs as novel photocatalysts to convert CO into solar fuels in nonaqueous media. Under AM 1.5G simulated illumination, the CsPbBr QDs steadily generated and injected electrons into CO, catalyzing CO reduction at a rate of 23.7 μmol/g h with a selectivity over 99.3%. Additionally, through the construction of a CsPbBr QD/graphene oxide (CsPbBr QD/GO) composite, the rate of electron consumption increased 25.5% because of improved electron extraction and transport. This study is anticipated to provide new opportunities to utilize halide perovskite QD materials in photocatalytic applications.
Heavy metal ions are highly toxic and widely spread as environmental pollutants. New strategies are being developed to simultaneously detect and remove these toxic ions. Herein, we take the intrinsic advantage of covalent organic frameworks (COFs) and develop fluorescent COFs for sensing applications. As a proof-of-concept, a thioether-functionalized COF material, COF-LZU8, was "bottom-up" integrated with multifunctionality for the selective detection and facile removal of mercury(II): the π-conjugated framework as the signal transducer, the evenly and densely distributed thioether groups as the Hg(2+) receptor, the regular pores facilitating the real-time detection and mass transfer, together with the robust COF structure for recycle use. The excellent sensing performance of COF-LZU8 was achieved in terms of high sensitivity, excellent selectivity, easy visibility, and real-time response. Meanwhile, the efficient removal of Hg(2+) from water and the recycling of COF-LZU8 offers the possibility for practical applications. In addition, X-ray photoelectron spectroscopy and solid-state NMR investigations verified the strong and selective interaction between Hg(2+) and the thioether groups of COF-LZU8. This research not only demonstrates the utilization of fluorescent COFs for both sensing and removal of metal ions but also highlights the facile construction of functionalized COFs for environmental applications.
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