- 标题
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- 实验方案
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Highly Sensitive and Selective Fluorescent Sensor based on a Multi-Responsive Ultrastable Amino-Functionalized Zn(II)-MOF for Hazardous Chemicals
摘要： A microscale amino-functionalized Zn(II)-MOF, namely [Zn(NH2-bdc)(4,4’-bpy)] (1) (NH2-H2bdc = 2-amino-1,4-benzenedicarboxylic acid and 4,4’-bpy = 4,4’-bipyridine), has been successfully synthesized, structurally characterized and further utilized as multi-responsive fluorescent sensor for highly sensitive and selective detection of Cr(VI) and 2,4,6-trinitrophenol (TNP). Compound 1 features non-porous 5-fold interpenetrated 3D framework with the Lewis basic sites including the uncoordinated amino and carboxylate groups on the framework for anchoring and recognizing the guest. 1 exhibits not only excellent water and thermal stability but also tolerance to acidic and basic media over an extensive pH range of 2-12. This ultrastable material can sensitively and selectively detect Cr2O7 2- and CrO4 2- in water based on the luminescent quenching with relatively low limits of detection (2.21 μM for CrO4 2- and 1.30 μM for Cr2O7 2-). Moreover, the unprecedented solvent-dependent luminescent response of 1 as a fluorescent probe for high-efficiency TNP detection was observed. Significantly, 1 not only displays high sensitive fluorescent enhancement upon TNP binding in ethanol but also exhibits fluorescent quenching toward TNP in water with very low limits of detection of 4.47 nM and 0.32 μM in ethanol and water, respectively. This work reports the first example of the utilization of MOF as a sensor for the detection of TNP based on dual responsive luminescence. Importantly, 1 can be simply and rapidly regenerated, displaying excellent recyclability after the sensing experiments.
关键词： Multi-responsive fluorescent sensors,Fluorescent quenching,Metal-organic framework,2,4,6-trinitrophenol,Fluorescent enhancement,Cr(VI)
更新于2025-11-19 16:46:39
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{Zn <sub/>6</sub> } Cluster Based Metal–Organic Framework with Enhanced Room-Temperature Phosphorescence and Optoelectronic Performances
摘要： Molecule-based solid-state materials with long lifetimes could enable longer migration distances for excitons, which are beneficial for vast applications in optoelectronic field. Herein, we report a hexanuclear zinc cluster based MOF exhibits highly enhanced phosphorescence about 2 orders of magnitude in comparison with the pristine phosphor ligand. The combination of both experimental and computational results suggest that the {Zn6} cluster is very important for adjusting molecular conformations, packing arrangement, and photophysical properties of the organic phosphor ligands within the MOF matrix. Optoelectronic measurements reveal that the MOF-modified electrode is catalytically active to hydrogen evolution under light irradiation in neutral solution. Thus, our study provide an effective way to achieve low-cost metal-based phosphorescence MOF, expanding its further optoelectronic applications.
关键词： optoelectronic performances,metal?organic framework,hexanuclear zinc cluster,room-temperature phosphorescence
更新于2025-11-14 15:23:50
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Metal ion induced single-crystal-to-single-crystal transformation and luminescent sensing properties of resorcin arene-based metal-organic frameworks
摘要： In this work, two new resorcin[4]arene-based metal-organic frameworks (MOFs), namely, [(CH3)2NH2][Zn3(HL)(L)(DMF)(H2O)2]·2H2O (1-Zn) and [(CH3)2NH2]2[Cd3(L)2(H2O)4]·2DMF·2H2O (2-Cd), have been synthesized under solvothermal conditions (H4L represents the resorcin[4]arene-based ligand). 1-Zn exhibits a layer structure, while 2-Cd shows a 3D motif. Remarkably, by immersing 1-Zn in an aqueous solution of Cu2+ ions, a new Cu(II)-MOF [Cu2(H2L)2(H2O)2]·3.5H2O (1-Cu) was achieved via a metal ion induced single-crystal-to-single-crystal (SCSC) transformation manner, involving generation of new metal-O bond and change of metal ion coordination geometry. Moreover, luminescent detection properties for Fe3+ ions and Cr2O7 2- ions were also investigated with 1-Zn and 2-Cd as luminescent sensors.
关键词： Resorcin[4]arene,Metal-exchanged phrase transformation,Metal-organic framework,Luminescent sensors
更新于2025-09-23 15:23:52
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Versatile Processing of Metal-Organic Framework-Fluoropolymer Composite Inks with Chemical Resistance and Sensor Applications
摘要： We report a new class of MOF inks with a water-repellent, photocurable fluoropolymer (PFPE) having up to 90 wt% MOF loading. These MOF inks enable to process various MOFs through spray coating, pen writing, stencil printing, and moulding at room temperature. Upon UV-curing, the hydrophobic PFPE matrix efficiently blocks water permeation but allows accessibility of chemicals into MOF pores, thereby freeing the MOF to perform its unique function. Moreover, by introducing functional MOFs we successfully demonstrated a water-tolerant chemosensor for a class of aromatic pollutants in water and a chemical-resistant thermosensor for visualizing temperature image. This approach would open up innumerable opportunities for those MOFs that are otherwise dormant.
关键词： MOF-polymer composite,Chemosensor,MOF processing,Thermosensor,Metal-Organic Framework,Chemical resistance
更新于2025-09-23 15:23:52
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Efficient photo-Fenton activity in mesoporous MIL-100(Fe) decorated with ZnO nanosphere for pollutants degradation
摘要： Metal-organic frameworks (MOFs) have received significant interest as a promising photocatalyst for environmental remediation due to its high surface area and porous nature. The small pores (<2 nm) in microporous MOFs help the adsorption of small molecules but limits diffusion and accessing of bigger molecules from MOF cavities, thus preventing their applications in some situation. The aim of this work is to fabricate mesoporous MOF composite with larger pore sizes (>2 nm) and open pore cavities that can provide right pathways for ingoing and outgoing of molecules during catalysis. Herein, we successfully report stable mesoporous MIL-100(Fe) loaded with ZnO NS by an in situ self-assembly method. The prepared samples were characterized by Brunauer–Emmett–Teller (BET) and N2 adsorption-desorption isotherm to study their surface area and porosity. The catalytic performance of mesoporous MIL-100(Fe) was approximately 2-3 order of magnitude more than that of microporous MIL-100(Fe). Such higher catalytic activity in mesoporous MIL-100(Fe) can be ascribed to its mesocellular structure which can improve the molecular diffusion and accessibility inside MOF channels. The charge separation efficiency and photo-Fenton activity of mesoporous MIL-100(Fe) can further be increased by introduction of certain amount of ZnO NS and H2O2. Moreover, the as synthesized sample shows higher photo-Fenton degradation efficiency at lower pH value with certain amount of H2O2. Lastly, the possible catalytic mechanism has been tentatively proposed. This study not only used for the pollutants degradation but also provide useful platform for the application of mesoporous MOFs as an efficient photo-Fenton activity to various other fields.
关键词： Metal-organic framework,ZnO,MIL-100(Fe),self-assembly,photo-Fenton,mesoporous
更新于2025-09-23 15:23:52
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Indocyanine green–encapsulated nanoscale metal–organic frameworks for highly effective chemo-photothermal combination?cancer therapy
摘要： Indocyanine green (ICG), as the only U.S. Food and Drug Administrationeapproved near-infrared (NIR) clinical agent, has been considered as an ideal light absorber for laser-mediated photothermal therapy (PTT) in cancer treatment. However, the practical applications of ICG are severely hampered by its poor aqueous stability, rapid body clearance, and low cellular uptake. To overcome these limitations, we herein report the successful example of integrating ICG into a zeolitic imidazolate framework (ZIF-8) to fabricate a novel nanoscale ICG@ZIF-8 hybrid material. Through a simple one-pot synthesis method, a high loading content of 20.6% can be achieved in the resultant ICG@ZIF-8. The photostability and tumor accumulation of ICG are notably promoted due to the protection of the framework, leading to enhanced photothermal conversion ef?ciency. Furthermore, we also discover, for the ?rst time, that the pH-triggered release of large amount of Zn2t from ZIF-8 in tumor acidic microenvironment also signi?cantly contributes to targeted killing of cancer cells. As a result of the combined PTT and chemotherapy, ICG@ZIF-8 exhibits greatly improved diagnostic ef?cacy for both in vitro and in vivo cancer therapy, leading to 91% tumor eradication in all the mice treated with ICG@ZIF-8 and NIR irradiation. Hematoxylin and eosin (H&E)estained slices show that no noticeable tissue damage is observed in major organs, indicating the safety of ICG@ZIF-8.
关键词： Cancer,Metal-organic framework,Chemotherapy,Indocyanine green,Photothermal therapy
更新于2025-09-23 15:23:52
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Metal–organic framework coated titanium dioxide nanorod array p–n heterojunction photoanode for solar water-splitting
摘要： This paper presents a p–n heterojunction photoanode based on a p-type porphyrin metal–organic framework (MOF) thin film and an n-type rutile titanium dioxide nanorod array for photoelectrochemical water splitting. The TiO2@MOF core–shell nanorod array is formed by coating an 8 nm thick MOF layer on a vertically aligned TiO2 nanorod array scaffold via a layer-by-layer self-assembly method. This vertically aligned core–shell nanorod array enables a long optical path length but a short path length for extraction of photogenerated minority charge carriers (holes) from TiO2 to the electrolyte. A p–n junction is formed between TiO2 and MOF, which improves the extraction of photogenerated electrons and holes out of the TiO2 nanorods. In addition, the MOF coating significantly improves the efficiency of charge injection at the photoanode/electrolyte interface. Introduction of Co(III) into the MOF layer further enhances the charge extraction in the photoanode and improves the charge injection efficiency. As a result, the photoelectrochemical cell with the TiO2@Co-MOF nanorod array photoanode exhibits a photocurrent density of 2.93 mA/cm2 at 1.23 V (vs. RHE), which is ~ 2.7 times the photocurrent achieved with bare TiO2 nanorod array under irradiation of an unfiltered 300 W Xe lamp with an output power density of 100 mW/cm2.
关键词： p–n junction,photoanode,titanium dioxide,metal-organic framework,water-splitting
更新于2025-09-23 15:23:52
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Solid-phase hot-pressing of POMs-ZIFs precursor and derived phosphide for overall water splitting
摘要： A facile solid-phase hot-pressing method was applied to prepare bimetallic phosphides on carbon cloth without binder as efficient electrocatalysts for water splitting. High-performance electrocatalyst with high performance for both hydrogen and oxygen evolution reaction is attracting considerable attention in recent years. However, most electrocatalysts are powders and require to deposit on conductive substrates with binders, leading to complicated steps and hindering the improvement of long-term stability. This work exhibits a solid-phase hot-pressing method to prepare polyoxometalates based zeolitic imidazolate frameworks (POMs-ZIFs) precursor on carbon cloth (CC) rapidly and mildly. After phosphidation treatment, nitrogen-doped graphitic carbon layers coated phosphide on CC (CoP/MoP@NC/CC) is synthesized. CoP/MoP@NC/CC has excellent electrocatalytic performance for water splitting due to the synergistic effect of CoP, MoP and as-formed oxide/hydroxide layers. It shows the low overpotentials of 94 mV for HER and 270 mV for OER at the current density of 10 mA cm-2 in alkaline medium, which is superior to most of the reported phosphide-based electrocatalysts. Notably, the ultra-high current density of 1000 mA cm-2 can be reached at the overpotentials of only 475 mV for HER and 657 mV for OER. As both cathode and anode for overall water splitting, CoP/MoP@NC can achieve the current density of 50 mA cm-2 at the cell voltage of 1.71 V. The solid-phase hot-pressing method ensures the tight and uniform growth of the fast nucleating and stable materials on substrate and applies for more electrochemical reactions.
关键词： phosphide,hot-pressing,HER,OER,metal-organic framework
更新于2025-09-23 15:23:52
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Solvent-free Method to Encapsulate Polyoxometalate into Metal-Organic Frameworks as Efficient and Recyclable Photocatalyst for Harmful Sulfamethazine Degrading in Water
摘要： Through a less-investigated in-situ hot-pressing synthesis method, the phosphotungstic acid H3PW12O40 (denoted as PW12) was rapidly incorporated into a metal-organic framework MFM-300(In) in a short time, affording novel PW12@MFM-300(In) composites. This solvent-free preparation process is not only environment-friendly but also energy/time-saving. The inclusion of PW12 in MFM-300(In) was demonstrated by different physical and chemical characterizations. It was interesting to find that PW12@MFM-300(In) as new heterocatalysts display synergistic activity for the visible-light-driven catalytic degradation of pharmaceutically active compound sulfamethazine (SMT). 4-PW12@MFM-300(In) with excellent robustness possesses the high removal efficiency of about 98% toward SMT within 2 h at room temperature, and can also be recycled multiple times for this catalytic process.
关键词： polyoxometalate,metal-organic framework,solvent-free,sulfamethazine,photocatalytic materials
更新于2025-09-23 15:23:52
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Photosensitizing single-site metal?organic framework enabling visible-light-driven CO2 reduction for syngas production
摘要： Photocatalytic CO2 reduction into syngas (CO and H2) is one of sustainable strategies for recycling CO2 into value-added products. Herein, a simple and effective two-step self-assembly process was developed to functionalize phosphorescent metal-organic framework (MOF) with single site catalyst. The resulting (Co/Ru)n-UiO-67(bpydc) supplied molecular platform to enable fast multielectron injection from photosensitizers (PSs) to Co-catalyst, leading to the first MOF-based composite photocatalyst for efficient syngas production with a yield of 13600 μmol·g?1 (H2 : CO = 2 : 1) in 16 h, 29.2-fold higher than that of its homogeneous counterpart. The H2/CO ratios can be well controlled by carefully adjusting the molar ratio of PS/catalyst in the MOF platform and the water content in the photocatalytic system. This work provides a prospective strategy for recycling CO2 into H2-rich syngas by merging PSs and single-site catalysts into a MOF platform.
关键词： Metal-organic framework,CO2 reduction,photosensitizer,photocatalyst,syngas
更新于2025-09-23 15:23:52