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Nanoscale Fluorescent Metal?Organic Framework Composites as a Logic Platform for Potential Diagnosis of Asthma
摘要： Asthma is a common chronic disorder, and the decreased hydrogen sulfide (H2S) production in the lung has been considered as an early detection biomarker for asthma. However, the detection of H2S in biological systems remains a challenge; because it requires the designed sensors to have the following features: nanoscale size, good biocompatibility, real-time detection, high selectivity/sensitivity, and good water stability. Here, we propose the potential of using nanoscale fluorescent metal?organic framework (MOF) composites Eu3+/Ag+@UiO-66-(COOH)2 (hereafter denoted as EAUC) as a logic platform for tentative diagnosis of asthma by detecting the biomarker H2S. This INHIBIT logic gate based on Eu3+@UiO-66-(COOH)2 (EUC) can be produced by choosing Ag+ and H2S as inputs and by monitoring the fluorescent signal (I615) as an output. Our fluorescent studies indicate that the EAUC exhibits excellent selectivity, extreme sensitivity (limit of detection: 23.53 μM), and real-time in situ detection of H2S. Further, MTT analysis in PC12 cells shows that the EAUC possesses low cytotoxicity and favourable biocompatibility that are suitable for the detection of biomarker H2S in vivo, as demonstrated by the successful detection of spiked H2S in the diluted serum samples. This work represents the possibility of using MOF-based logic platform for tentative diagnosis of asthma in clinical medicine.
关键词： metal?organic frameworks,logic gate,asthma,chemical sensing,hydrogen sulfide
更新于2025-09-23 15:22:29
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Dual Quenching Electrochemiluminescence Strategy Based on 3D Metal-organic Frameworks for Ultrasensitive Detection of Amyloid-β
摘要： We have proposed a dual quenching electrochemiluminescence (ECL) strategy which based on Ru(bpy)3 2+ as chromophores caged in 3D Zn-oxalate metal-organic frameworks (Ru(bpy)3 2+/Zn-oxalate MOFs) for ultrasensitive detection of amyloid-β (Aβ). The three-dimensional chromophore connectivity in Zn-oxalate MOFs provided a network for rapid excited state energy transfer migration among Ru(bpy)3 2+ units which shielded the chromophores from solvent molecules and led to a high energy Ru emission efficiency. In addition, we found that both Au nanoparticles and NiFe-based nanocube MOFs could contribute to the reduction of the ECL intensity of chromophore. And the ECL emission spectra of 3D Ru(bpy)3 2+/Zn-oxalate MOFs overlapped appropriately with the ultraviolet visible (UV-vis) absorption spectra of Au@NiFe-MOFs composites, which could trigger the resonance energy transfer (RET) behavior between Ru(bpy)3 2+/Zn-oxalate MOFs (donor) and Au@NiFe-MOFs (acceptor), achieving the dual quenching effect of Ru(bpy)3 2+ encapsulated in 3D Zn-oxalate MOFs and significantly boosting the sensitivity of the Aβ-detection immunosensor. In order to examine the clinical practicability, we have applied it to verify the content of Aβ solution ranging from 100 fg mL-1 to 50 ng mL-1 and obtained the calibration cure with high correlation coefficient, along with the low limit of detection of 13.8 fg mL-1. Above all, this work demonstrated an approach of constructing dual quenching effect ECL immunosensors in whole 3D MOFs system and its application in ECL methodology.
关键词： Ru(bpy)3 2+,Dual quenching electrochemiluminescence,Au@NiFe nanocube,3D Zn-oxalate metal-organic frameworks,Amyloid-β detection
更新于2025-09-23 15:22:29
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Monometallic Catalytic Models Hosted in Stable Metal-Organic Frameworks for Tunable CO2 Photoreduction
摘要： The photocatalytic reduction of CO2 to energy carriers has emerged as one of the most promising strategy to alleviate the energy crisis and CO2 pollution, for which the development of catalyst was considered as the determining factor for the accomplishment of this conversion process. In this study, three stably and isostructural metal organic frameworks (denoted as MOF-Ni, MOF-Co and MOF-Cu), have been synthesized and used as heterogeneous catalysts applied into photocatalytic CO2 reduction reaction (CO2RR). It is worth noting that the MOF-Ni exhibited a very high selectivity of 97.7% for photoreducing CO2 to CO, which has exceeded most of the reported MOF-based catalysts in the field. Significantly, the MOFs associated with monometallic catalytic centre offer a simply and precisely structural model which allows us to understand the specific effects of different metal ion species on photoreduction of CO2 as well as reactive mechanism more intuitively.
关键词： Isostructural,Metal-Organic Frameworks,Photocatalytic CO2 Reduction,High Selectivity,Monometallic Catalytic Model,Reactive Mechanism
更新于2025-09-23 15:22:29
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The Transitional Transmittance Response of ZIF-8 Gas Adsorption Observed Using Terahertz Waves
摘要： In this study, we recorded the transitional response in terms of terahertz transmittance of zeolitic imidazole framework-8 [Zn(2-methylimidazolate)2, ZIF-8] at 2.0 THz as a function of exposure time to gaseous propane and n-butane. The transmittance at 2.0 THz increased as gas adsorbed onto the ZIF-8. Conversely, during a nitrogen purge, transmittance decreased as the alkane gas desorbed. We estimated time constants for the adsorption and desorption of the two gases by comparing the plots of their responses. We also demonstrated the potential of using a combination of ZIF materials and terahertz technology as a novel gas analyzer.
关键词： Adsorption kinetics,Terahertz vibration,Metal-organic frameworks,Porous solids,Infrared absorption spectroscopy
更新于2025-09-23 15:22:29
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Dynamic Nuclear Polarization of Metal–Organic Frameworks Using Photoexcited Triplet Electrons
摘要： While dynamic nuclear polarization based on photoexcited triplet electrons (triplet-DNP) has the potential to hyperpolarize nuclear spins of target substrates in the low magnetic field at room temperature, there has been no triplet-DNP system offering structural rigidity and substrate accessibility. Here, we report the first example of triplet-DNP of nanoporous metal?organic frameworks. Accommodation of a carboxylate-modified pentacene derivative in a partially deuterated ZIF-8 (D-ZIF-8) results in a clear 1H NMR signal enhancement over thermal equilibrium.
关键词： dynamic nuclear polarization,photoexcited triplet electrons,metal?organic frameworks,NMR signal enhancement
更新于2025-09-23 15:21:21
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Ratiometric Luminescent Sensor of Picric Acid based on the Dual-Emission Mixed-Lanthanide Coordination Polymer
摘要： Powerful explosive sensors play a key role in public security and environmental protection. Herein we report a series of isostructural lanthanide coordination polymers [Ln2L1.5(NMP)2]n (LnL, Ln = Eu , Gd, Tb, Dy, Ho and Er, H4L = [1,1′:4′,1″-terphenyl]-2′,4,4″,5′-tetracarboxylic acid, NMP = N-methyl-2-pyrrolidone) and mixed-Ln LnL (EuxTb1-xL, EuxGd1-xL, TbxGd1-xL and EuxTb0.02-xGd0.98L). Luminescence studies show that both H4L and GdL emit strong fluorescence and phosphorescence at 77 K while only fluorescence at room temperature, and TbL exhibits strong Tb3+ characteristic emission though the energy difference between the triplet excited state of H4L (20661 cm-1) and the 5D4 energy level of Tb3+ (20500 cm-1) is very small. By doping Eu3+ and Tb3+ into GdL, we obtained EuxTb0.02-xGd0.98L emitting warm white light. For TbL and Tb0.01Gd0.99L showing the dual-emission, upon addition of picric acid (PA) into their suspensions in Tris-HCl buffer, Tb3+ emission decreases slowly, however, the ligand-based emission is sharply quenched, rendering TbL and Tb0.01Gd0.99L excellent single-lanthanide and mixed-lanthanide ratiometric luminescence PA sensor materials, respectively.
关键词： picric acid (PA),ratiometric luminescence sensors,white light emission,metal-organic frameworks (MOFs),Coordination polymers (CPs)
更新于2025-09-23 15:21:21
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Engineering Metal Organic Frameworks for Photoacoustic Imaging Guided Chemo/Photothermal Combinational Tumor Therapy
摘要： Imaging-guided therapy has considerable potential in tumor treatment. Different treatments have been integrated to realize combinational tumor therapy with improved therapeutic efficiency. Herein, the conventional metal organic framework (MOF) MIL-100 is utilized to load curcumin with excellent encapsulation capacity. Polydopamine-modified hyaluronic acid (HA-PDA) is coated on MIL-100 surface to construct engineering MOF nanoparticles (MCH NPs). The HA-PDA coating not only improves the dispersibility and stability of NPs but also introduces a tumor-targeting ability to this nanosystem. A two-stage augmented photothermal conversion capability is introduced to this nanosystem by encapsulating curcumin in MIL-100 pores and then coating HA-PDA on the surface, which confer the MCH NPs with strong photothermal conversional efficiency. After being intravenously injected into xenograft HeLa tumor-bearing mice, MCH NPs prefer to accumulate at the tumor site and achieve photoacoustic imaging-guided chemo/photothermal combinational tumor therapy, generating nearly complete tumor ablation. Engineering MOFs is an efficient platform for imaging-guided combinational tumor therapy, as confirmed by in vitro and in vivo evaluations.
关键词： curcumin,photoacoustic imaging,metal organic frameworks,chemotherapy,photothermal therapy
更新于2025-09-23 15:21:21
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Design of lanthanide-based metal-organic frameworks with enhanced near-infrared emission
摘要： A strategy based on the use of ligand steric hindrance and metal doping is reported for the design and synthesis of near-infrared (NIR) emitting lanthanide-based metal–organic frameworks (MOFs). The lanthanide ions are free of coordinated solvents, and the resulting NIR-MOFs are highly emissive and exhibit long luminescence lifetimes.
关键词： metal doping,ligand steric hindrance,lanthanide-based metal–organic frameworks,luminescence,near-infrared emission
更新于2025-09-23 15:21:01
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Preparation and Characterization of Metal-Organic Frameworks and its Composites Eu <sub/>2</sub> O <sub/>3</sub> @[Zn <sub/>2</sub> (bdc) <sub/>2</sub> dabco] (ZBDh) via Pulsed Laser Ablation in Flow Liquid
摘要： This work reports the compounds of [Zn2(bdc)2dabco] (ZBDh) and [Zn2(bdc)2dabco] (ZBDt) and the composite Eu2O3@[Zn2(bdc)2dabco](ZBDh) synthesized by pulsed laser ablation in flowing liquid. At an appropriate reactants concentration of reactants, the phase ZDBh transforms into phase ZDBt by an increase of the irradiation time from 4 to 40 mins. The results show that the Eu2O3 nanoparticles with an average size of 3.17 nm are uniformly distributed among the crystal and the BET specific surface area of the composite Eu2O3@[Zn2(bdc)2dabco] (ZBDh) is 1621 m2/g, which is larger than that of compound [Zn2(bdc)2dabco] (ZBDh). Moreover, the composite Eu2O3@[Zn2(bdc)2dabco](ZBDh) can emit very intense characteristic fluorescence at 613 nm of Eu3+ ion under ultraviolet radiation and can be used for detecting of methanol molecules in fluorescence sensing because of its fluorescence intensity at 613 nm is sensitive to the content of methanol in solvent.
关键词： pulsed laser ablation,metal-organic frameworks,Eu2O3 nanoparticles,fluorescence sensing,methanol detection
更新于2025-09-23 15:21:01
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Rapid Generation of Hierarchically Porous Metal-Organic Frameworks through Laser Photolysis
摘要： Hierarchically porous metal–organic frameworks (HP-MOFs) facilitate mass transfer due to mesoporosity while preserving the advantage of microporosity. This unique feature endows HP-MOFs with remarkable application potential in multiple fields. Recently, new methods such as the construction of HP-MOFs have emerged. To further enrich the synthetic toolkit of MOFs, we report a controlled photolytic removal of linkers to create mesopores within microporous MOFs at tens of milliseconds. Ultraviolet (UV) laser has been applied to eliminate “photolabile” linkers without affecting the overall crystallinity and integrity of the original framework. Presumably, the creation of mesopores can be attributed to the missing-cluster defects, which can be tuned through varying the time of laser exposure and ratio of photolabile/robust linkers. Upon laser exposure, MOF crystals shrank while metal oxide nanoparticles formed giving rise to the HP-MOFs. In addition, photolysis can also be utilized for the fabrication of complicated patterns with high precision, paving the way towards MOF lithography, which has enormous potential in sensing and catalysis.
关键词： linker photolysis,metal-organic frameworks,hierarchical pores
更新于2025-09-23 15:21:01