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Here, SnS2/polypyrrole (PPy) was synthesized, which shows high catalytic activity for the photocatalytic oxidation of benzylamine under mild conditions (at 25 °C, in air and without adding an additional sacrificial reagent, redox mediator and photosensitizer).
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Low-dimensional metal-organic frameworks (MOFs) exhibit enhanced properties compared with three-dimensional (3D) geometry MOFs in many fields. In this work, we demonstrate the synthesis of Cu3(BTC)2 (BTC = benzene-1,3,5-tricarboxylate) nanoflakes in a binary solvent of ionic liquid (IL) and water. Such a MOF architecture has a high surface area and abundant unsaturated coordination metal sites, making them attractive for adsorption and catalysis. For example, in catalyzing the oxidation reactions of a series of alcohols, the Cu3(BTC)2 nanoflakes exhibit a high performance that is superior to Cu3(BTC)2 microparticles synthesized in a conventional solvent. Experimental and theoretical studies reveal that the IL accelerates the crystallization of Cu3(BTC)2, while water plays a role in stripping the Cu3(BTC)2 blocks that are formed at an early stage through its attack on the crystal plane of Cu3(BTC)2. Such an in situ crystallization-exfoliation process that uses an IL/water solvent opens a new route for producing low-dimensional MOFs.
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To improve the photocatalytic performance of metal-organic frameworks is of great importance. We synthesized the nanosheets of a zeolitic imidazolate framework (ZIF-9(III)) in ionic liquid/ethanol solution, with an average thickness of 4.6 nm. The as-synthesized ZIF-9(III) nanosheets have optoelectronic properties superior to the three-dimensional ZIF-9(III) synthesized by the conventional solvothermal method. The ZIF-9(III) nanosheets exhibit high activity for photocatalytic hydrogen production under visible light irradiation. The maximum hydrogen production rate can reach 112.37 mmol g-1 h-1, while that by three-dimensional ZIF-9(III) is 29.64 mmol g-1 h-1 under the same experimental conditions.
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The development of highly catalytic hydrogen-bonded organic frameworks (HOFs) is of great importance, but remains challenging. Herein, we demonstrate the fabrication of a periodically nanoporous HOF for high performance photocatalysis. Compared with the conventional microporous HOFs, the nanoporous HOF architecture has a larger number of free carboxyl groups on the surface and presents greatly improved photoelectrochemical properties. It exhibits high catalytic activity for the photo-oxidative coupling of amines under mild conditions such as air atmosphere and room temperature and without any co-catalysts, sacrificial reagents or photosensitizers. The relationship between the structure, properties and catalytic performance of the nanoporous HOF was studied by experimental and theoretical investigations. It shows that such a HOF structure facilitates reactant adsorption and O2 dissociation, thus promoting the oxidative coupling reaction. This work provides a new way for improving the catalytic performance of a single HOF.
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Herein, we demonstrated a highly efficient photocatalytic sulfide oxidation reaction at ambient conditions without a sacrificial reagent or redox mediator, by using Co(NO3)2/covalent organic framework nanoparticles as a photocatalyst.
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Electrochemical conversion of CO2 to valuable fuels is appealing for CO2 fixation and energy storage. The Cu-based catalysts feature unique superiorities, but achieving high ethylene selectivity is still restricted. In this study, we propose the anchoring of an ionic liquid (IL) on a Cu electrocatalyst for improving the electrochemical CO2 reduction to ethylene. In a water-based electrolyte and a commonly used H-type cell, a high ethylene Faradaic efficiency of 77.3 % was achieved at -1.49â V (vs. RHE). Experimental and theoretical studies reveal that an IL can modify the electronic structure of a Cu catalyst through its interaction with Cu, making it more conducive to *CO dimerization for ethylene formation.
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Pickering emulsion is a heterogeneous system consisting of at least two immiscible liquids, which are stabilized by solid particles, in which organic solvent or water is dispersed into other phase in form of micrometre-sized droplets. Compared to traditional emulsions stabilized by surfactant, solids are cheap and can be easily separated and recycled by centrifugation or filtration after use. Moreover, the properties of Pickering emulsions can be adjusted by using different types of solid particles. Up to now, Pickering emulsions have been applied in a wide range of areas such as material science and catalysis. Here we review recent studies on Pickering emulsions stabilized by metal-organic framework, graphitic carbon nitride and graphene oxide.
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The macro-meso-microporous and defective metal-organic framework constructed by transition metal Zn and 2,2'-bipyridine-5,5'-carboxylate was synthesized in CO2-expanded solvent. It shows high photocatalytic activity and selectivity for the oxidation of amines to imines under mild conditions, i.e., air as an oxidant, room temperature, and involving no photosensitizer or cocatalyst.