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Selective Photooxidation of Amines and Sulfides Triggered by a Superoxide Radical Using a Novel Visible-Light-Responsive Metal–Organic Framework
摘要： Photocatalysis is an efficient and sustainable approach to convert solar energy into chemical energy, simultaneously supplying valuable chemicals. In this study, a novel metal–organic framework (MOF) compound is constructed from anthracene-based organic linkers, which shows visible-light absorption and efficient photoinduced charge generation property. It was applied for triggering photooxidation of benzylamines and sulfides in the presence of environmental benign oxidants of molecular oxygen or hydrogen peroxide. Results show that it is a highly selective photocatalyst for oxidation reactions to produce valuable imines or sulfoxides. We further investigate the underlying mechanism for these photocatalytic reactions by recognizing reactive oxygen species in the reactions. It has been demonstrated that the superoxide radical (O2??), generated by electron transfer from a photoexcited MOF to oxidants, serves as the main active species for the oxidations. The work demonstrates the great potential of photoactive MOFs for the transformation of organic chemicals into valuable complexes.
关键词： sulfide,photocatalysis,metal–organic framework,benzylamine,oxidation
更新于2025-09-23 15:23:52
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A unique (4,4,5)-connected 3D zinc (II) metal-organic framework for highly efficient photodegradation of Rhodamine B under UV light
摘要： A new zinc (II) metal-organic framework, [Zn3(L)2(nbta)2]n (1) (L = 1,4-bis(benzimidazol-1-yl)-2-butene, H3nbta = 5-nitro-1,2,3-benzenetricarboxylic acid) was hydrothermally synthesized and structural characterized. 1 possesses a unique 3D (4,4,5)-connected network with a Schl?fla symbol of {42.63.8}2{44.62}{47.63}2. Furthermore, the photocatalytic property of 1 for degradation of the Rhodamine B (RhB) was examined under UV irradiation.
关键词： Semi-rigid bis(benzimidazole),Hydrothermal synthesis,Crystal structure,Metal-organic framework,Zinc (II),Photocatalytic degradation
更新于2025-09-23 15:22:29
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Influence of operational parameters on the photocatalytic performance of DE-NOx process Via MIL-101(Fe)
摘要： Metal organic framework (MOF) has been paid great attention as a potential candidate for various applications in the field of energy and environment, particularly in air purification. Among various MOFs, MIL-101(Fe) represents an interesting material possessing many advantages, including the ease of fabrication, high porosity, high specific surface area with open metal sites, making it a promising material in the field of harmful gas treatment. Taking these advantages, MIL-101(Fe) was synthesized by facile microwave-solvothermal method and applied as a photocatalyst for the degradation of NOx. The de-NOx efficiency of the synthesized powder was evaluated with respect to various operating parameters including substrates, sample doses, light spectrum and light intensity, initial NO concentration, and relative humidity. The results have shown that the efficiency of NOx photocatalytic degradation reaches to 77% under solar irradiation via 0.1 g of MIL-101(Fe) with optimum condition of reaction, (alumina substrate, 350 ppb of initial NO concentration, 40–50% of relative humidity). Then this work provides the optimum condition for the efficient photocatalytic degradation of NOx.
关键词： Gaseous pollutant,Metal-organic framework,Photocatalyst,NOx emission,MIL-101
更新于2025-09-23 15:22:29
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Metal-Organic Frameworks Derived from Zero-Valent Metal Substrates: Mechanisms of Formation and Modulation of Properties
摘要： The replicative construction of metal–organic frameworks (MOFs) templated with solvent-insoluble solid substrates is of marked importance, as it allows for the assembly of 2D and 3D macro- and mesoscopic architectures with properties that are challenging to attain by the conventional solution-based synthesis approach. This work reports an in situ and direct construction of MOFs from zero-valent metal substrates via a green hydrothermal oxidation–MOF construction chemistry without the use of any additional metal source, chemical reagents, or acidification of solvent, and elucidates the zero-valent metal derived formation mechanisms of MOFs and their structure modulation to 1D nanofibers (NFs), 2D film, and 3D core–shell microstructures. Through modulation of the competing surface oxidation-dissolution and MOF crystallization kinetics, Al@MIL-53 core–shell microstructures and MIL-53 (Al) NFs are obtained that exhibit unique morphologies and marked properties superior to the conventional MIL-53 (Al) powders. The generality of zero-valent metal-templated synthesis of MOFs is demonstrated with formation of MIL-53 (Al), HKUST-1, and ZIF-7 polycrystalline films on Al, Cu, and Zn metal meshes, elucidating the significance of the approach utilizing solid metal substrate that can be easily processed into various shapes, architectures, and compositions.
关键词： MOF nanofibers,formation mechanism,core–shell structure,templated synthesis,metal–organic framework
更新于2025-09-23 15:22:29
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White-Light-Emitting Decoding Sensing for Eight Frequently-Used Antibiotics Based on a Lanthanide Metal-Organic Framework
摘要： Developing multi-selective luminescence sensing technology to differentiate serial compounds is very important but challenging. White-light-emitting decoding sensing based on lanthanide metal-organic frameworks (Ln-MOFs) is a promising candidate for multi-selective luminescence sensing application. In this work, three isomorphic Ln-MOFs based on H3dcpcpt (3-(3,5-dicarboxylphenyl)-5-(4-carboxylphenl)-1H-1,2,4-triazole) ligand, exhibiting red, blue, and green emission, respectively, have been synthesized by solvothermal reactions. The isostructural mixed Eu/Gd/Tb-dcpcpt is fabricated via the in-situ doping of different Ln3+ ions into the host framework, which can emit white light upon the excitation at 320 nm. It is noteworthy that this white-light-emitting complex could serve as a convenient luminescent platform for distinguishing eight frequently-used antibiotics: five through luminescence-color-changing processes (tetracycline hydrochloride, yellow; nitrofurazone, orange; nitrofurantoin, orange; sulfadiazine, blue; carbamazepine, blue) and three through luminescence quenching processes (metronidazole, dimetridazole, and ornidazole). Moreover, a novel method, 3D decoding map, has been proposed to realize multi-selective luminescence sensing applications. This triple-readout map features unique characteristics on luminescence color and mechanism. The mechanism has been systematically interpreted on the basis of the structural analysis, energy transfer and allocation process, and peak fitting analysis for photoluminescence spectra. This approach presents a promising strategy to explore luminescent platforms capable of effectively sensing serial compounds.
关键词： lanthanide,metal-organic framework,multi-selective luminescence sensing,decoding sensing,white light,antibiotics
更新于2025-09-23 15:22:29
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Highly Photostable and Fluorescent Microporous Solids Prepared via Solid-state Entrapment of BODIPY Dyes in a Nascent Metal-Organic Framework
摘要： We report a strategy to synthesize highly emissive, photostable, microporous materials by solid-state entrapment of boron dipyrromethene (BODIPY) fluorophores in a metal-organic framework. Solvent-free mechanochemistry or accelerated aging enabled quantitative capture and dispersal of the PM605 dye within the ZIF-8 framework starting from inexpensive, commercial materials. While the design of emissive BODIPY solids is normally challenged by quenching in a densely-packed environment, herein reported PM605@ZIF-8 materials show excellent emissive properties and to the best of our knowledge an unprecedented ~10-fold enhancement of BODIPY photostability. Time-resolved and steady-state fluorescence studies of PM605@ZIF-8 show that interchromophore interactions are minimal at low dye loadings, but at higher ones through-pore energy transfer between chromophores and to aggregate species lead to quenching.
关键词： fluorescence,metal-organic framework,photostability,BODIPY,microporous materials
更新于2025-09-23 15:21:21
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Selective and Sensitive Sensing of Hydrogen Peroxide by a Boronic Acid Functionalized Metal–Organic Framework and Its Application in Live-Cell Imaging
摘要： A new boronic acid functionalized Zr(IV) metal?organic framework having the capability of sensing H2O2 in live cells is reported. The Zr-MOF bears a UiO-66 structure and contains 2-boronobenzene-1,4-dicarboxylic acid (BDC-B(OH)2) as a framework linker. The activated Zr-UiO-66-B(OH)2 compound (called 1′) is highly selective for the ?uorogenic detection of H2O2 in HEPES bu?er at pH 7.4, even in the presence of interfering ROS (ROS = reactive oxygen species) and other biologically relevant analytes. The ?uorescent probe was found to display extraordinary sensitivity for H2O2 (detection limit 0.015 μM) in HEPES bu?er, which represents a lower value in comparison to those of the MOF probes documented so far for sensing H2O2 using other analytical methods. Taking advantage of its high selectivity and sensitivity for H2O2 in HEPES bu?er, the probe was successfully employed for the imaging of intracellular H2O2. Imaging studies with MDAMB-231 cells revealed the emergence of bright blue ?uorescence after loading with probe 1′ and subsequent treatment with H2O2 solution.
关键词： Zr(IV) metal?organic framework,boronic acid,live-cell imaging,fluorescent probe,H2O2 sensing
更新于2025-09-23 15:21:21
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Semiconducting Langmuir-Blodgett Films of Porphyrin Paddle-Wheel Frameworks for Photoelectric Conversion
摘要： Understanding the photocurrent transportation within porphyrin-containing metal-organic frameworks (PMOFs) will be a critical step for applying these materials in light-harvesting molecular devices in the future. Two copper porphyrin paddle-wheel frameworks (Cu-PPFs) were employed to study the influence of metal ions coordinated into the porphyrin ligands on conductivity and photoelectron transfer capability. To compare the electronic and optical properties of both materials, we prepared an ultra-thin film of each PPF via a Langmuir-Blodgett method. The resulting films exhibited uniform morphology and single-crystalline domains, in addition to photoelectric conversion capabilities. We confirmed both Cu-PPFs have semiconducting properties with an optical bandgap around 2.7 eV. The current density generated by both Cu-PPFs were studied through a mercury drop junction approach. We observed a slightly higher conductivity from the Cu-PPF film consisting of metalloporphyrins than the one without copper doping in the porphyrin centers. In addition, the copper ions coordinated porphyrins were found to be more favorable for facilitating photo-induced electron transfer from the Cu-PPF film to a conductive glass substrate. This work presents a new approach of combining thin film fabrication and electro-heterojunction measurement to study electron transfer within an ultra-thin film.
关键词： Metal-Organic Framework (MOF),2D Material,Langmuir-Blodgett Film,Self-Assembly,Semiconductor,Porphyrin Thin Film,Photoelectric Conversion
更新于2025-09-23 15:21:21
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Heterojunction Incorporating Perovskite and Microporous Metala??Organic Framework Nanocrystals for Efficient and Stable Solar Cells
摘要： In this paper, we present a facile approach to enhance the efficiency and stability of perovskite solar cells (PSCs) by incorporating perovskite with microporous indium-based metal–organic framework [In12O(OH)16(H2O)5(btc)6]n (In-BTC) nanocrystals and forming heterojunction light-harvesting layer. The interconnected micropores and terminal oxygen sites of In-BTC allow the preferential crystallization of perovskite inside the regular cavities, endowing the derived films with improved morphology/crystallinity and reduced grain boundaries/defects. Consequently, the In-BTC-modified PSC yields enhanced fill factor of 0.79 and power conversion efficiency (PCE) of 20.87%, surpassing the pristine device (0.76 and 19.52%, respectively). More importantly, over 80% of the original PCE is retained after 12 days of exposure to ambient environment (25 °C and relative humidity of ~ 65%) without encapsulation, while only about 35% is left to the pristine device.
关键词： Light-harvesting layer,Metal–organic framework,Heterojunction,Perovskite solar cell,Nanocrystal
更新于2025-09-23 15:21:01
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An ultrasensitive luteolin sensor based on MOFs derived CuCo coated nitrogen-doped porous carbon polyhedron
摘要： Designing high-efficiency electrocatalysts for luteolin detection is essential and vital in biological and medical field. Herein, CuCo coated nitrogen-enriched porous carbon polyhedron (CuCo@NPCP) materials are fabricated as a highly sensitive electrochemical luteolin sensor by simple and mild approach. As characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption-desorption isotherms and electrochemical methods, CuCo@NPCP materials possess high specific surface area, 3D porous framework, amounts of available active sites, which all contribute to the adsorption and catalysis for luteolin. Meanwhile, vast mesoporous structure of CuCo@NPCP further affords more mass transport channels and enhances the mass transfer capacity. Thanks to above-mentioned characteristics, optimal Cu1Co3@NPCP presents superior analytical performance: a wide linear range from 0.2 nM to 2.5 μM, a ultrahigh sensitivity of 134.57 μA μM-1 surpassing to other reported catalysts previously, a low detection limit of 0.08 nM, as well as satisfactory selectivity, reproducibility, and long-term stability. This work offers an attractive catalyst derived from MOFs for constructing effective luteolin sensors.
关键词： Luteolin sensor,Metal-organic framework derivatives,Ultrahigh sensitivity,Trace detection
更新于2025-09-23 15:21:01