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- 摘要
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- 实验方案
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Circularly Polarized Rooma??Temperature Phosphorescence and Encapsulation Engineering for MOFa??Based Fluorescent/Phosphorescent WLEDs
摘要： Optical materials with circularly polarized luminescence and room temperature phosphorescence currently attract great attention owing to their unique optoelectronic properties. Herein, via the coordination-induced assembly strategy, a homochiral metal–organic framework (MOF) 1 with high stability and porosity is successfully synthesized by using the achiral triphenylamine-based molecule as the building block. Remarkably, MOF 1 shows circularly polarized luminescence and phosphorescence at room temperature simultaneously, also with excellent anisotropic optical properties. Furthermore, MOF 1 can serve as a nanocontainer to construct dye-encapsulated host–guest systems. Importantly, the multicolor emissions including white-light emission can be achieved. The corresponding color rendering index and correlated color temperature values of light emitting device are 73 and 5541 K, when using dye-loaded MOF 1?RhB 10 (CIE: 0.33, 0.33) as single-phase white light-emitting phosphor. This study first reports circularly polarized phosphorescence based on MOF without precious metals under ambient conditions, and also is first time for phosphorescent polarized materials with high porosity. These results will open up a new pathway to the design of porous chiroptical materials and white-light materials.
关键词： circularly polarized luminescence,host–guest system,room temperature phosphorescence,white light emitting devices,metal–organic frameworks
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
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Higha??Performance Methanal Sensor Based on Metala??Organic Framework Based Onea??Dimensional Photonic Crystal
摘要： One-dimensional photonic crystal (1DPC) based on metal-organic framework (MOF) (MIL-101-NH2 (Cr) / TiO2)n was prepared by a spin coating method. The 1DPC structure was built to detect vapor gas. The optical properties of the 1DPC were investigated by varying the number of period, incident angles and thickness of MOF, and the results of the experiment are agreed with theoretical simulation. The 1DPC gas sensor shows good selectivity for vapor gas and allows for a reliable distinction between methanal and other investigated analytes with the maximal peak shift (43 nm). It was found that the response time and recovery time for the sensor are around 500 ms and 20 s, respectively. The relationship between the peak shift position and the methanal concentration was demonstrated to be linear. Moreover, the fabricated 1DPC exhibited high repeatability and long-term storage and thermal stability, which are beneficial for practical applications.
关键词： Sensors,Nanostructures,Metal-organic frameworks,Photonic Crystal
更新于2025-09-23 15:21:01
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Coupled Electrical Conduction in Coordination Polymers: From Electrons/Ions to Mixed Charge Carriers
摘要： The coupled transport of ions and electrons is of great potential for next-generation sensors, energy storage and conversion devices, optoelectronics, etc. Coordination polymers (CPs) intrinsically have both transport pathways for electrons and ions, however, the practical conductivities are usually low. In recent years, significant advances have been made in electronic or ionic conductive coordination polymers, which also results in progress in mixed ionic-electronic conductive coordination polymers. Here we start from electronic and ionic conductive CPs to mixed ionic-electronic conductive CPs. Recent advances in the design of mixed ionic-electronic conductive CPs are summarized. In addition, devices based on mixed conduction are selected.
关键词： metal-organic frameworks,coordination polymers,ionic,conductivity,electronic
更新于2025-09-23 15:19:57
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Visible-Light-Driven Rotation of Molecular Motors in a Dual-Function Metala??Organic Framework Enabled by Energy Transfer
摘要： The visible-light driven rotation of an overcrowded-alkene based molecular motor strut in a dual-function metal-organic framework (MOF) is reported. Two types of functional linkers, a palladium-porphyrin photosensitizer and a bispyridine derived molecular motor were used to construct the framework capable of harvesting low-energy green light to power the rotary motion. The molecular motor was introduced in the framework using the post synthetic solvent assisted linker exchange (SALE) method and the structure of the material was confirmed by powder (PXRD) and single crystal X-ray (SC-XRD) diffraction. The large decrease in the phosphorescence lifetime and intensity of the porphyrin in the MOFs upon introduction of the molecular motor pillars confirms efficient triplet-to-triplet energy transfer between the porphyrin linkers and molecular motor. Near infrared Raman spectroscopy revealed that the visible light driven rotation of the molecular motor proceeds in the solid state at rates similar to those observed in solution.
关键词： molecular motors,metal-organic frameworks,molecular machines,energy transfer
更新于2025-09-23 15:19:57
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Ultrathin two-dimensional conjugated metala??organic framework single-crystalline nanosheets enabled by surfactant-assisted synthesis
摘要： Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have recently emerged for potential applications in (opto-)electronics, chemiresistive sensing, and energy storage and conversion, due to their excellent electrical conductivity, abundant active sites, and intrinsic porous structures. However, developing ultrathin 2D c-MOF nanosheets (NSs) for facile solution-processing and integration into devices remains a great challenge, mostly due to unscalable synthesis, low yield, limited lateral size and low crystallinity. Here, we report a surfactant-assisted solution synthesis toward ultrathin 2D c-MOF NSs, including HHB-Cu (HHB=hexahydroxybenzene), HHB-Ni and HHTP-Cu (HHTP=2,3,6,7,10,11-hexahydroxytriphenylene). For the first time, we achieve single-crystalline HHB-Cu(Ni) NSs featured with a thickness of 4-5 nm (~8-10 layers) and a lateral size of 0.25-0.65 μm2, as well as single-crystalline HHTP-Cu NSs with a thickness of ~5.1±2.6 nm (~10 layers) and a lateral size of 0.002-0.02 μm2. Benefiting from the ultrathin feature, the synthetic NSs allow fast ion diffusion and high utilization of active sites. As a proof of concept, when serving as a cathode material for Li-ion storage, HHB-Cu NSs deliver a remarkable rate capability (charge within 3 min) and long-term cycling stability (90% capacity retention after 1000 cycles), superior to the corresponding bulk materials and other reported MOF cathodes.
关键词： Li-ion batteries,Two-dimensional conjugated metal-organic frameworks,electrochemical performance,surfactant-assisted synthesis,ultrathin nanosheets
更新于2025-09-23 15:19:57
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Gold nanoparticles doped metal-organic frameworks as near-infrared light-enhanced cascade nanozyme against hypoxic tumors
摘要： We report gold nanoparticles (AuNPs) doped iron-based metal-organic frameworks (GIM) which displays near-infrared light (NIR)-enhanced cascade nanozyme against hypoxic tumors. Due to the strong protein adsorption-induced surface passivation, AuNPs suffer from the loss of glucose oxidase (GOx) activity. However, GIM could protect the GOx-like activity of AuNPs with the satisfactory shield capability. In addition, GIM exhibited excellent photothermal conversion ability and unique NIR light-enhanced GOx-like activity, which could efficiently increase the endogenous H2O2 production. Meanwhile, as the produced H2O2 is converted by GIM into O2 and highly toxic (cid:1668)OH. Thus, GIM-catalyzed cascade reactions with NIR light irradiation not only offer the O2 but also promote the reactive oxygen species (ROS) generation at tumor sites. The produced O2 could be further applied to AuNPs catalytic oxidation of glucose and relieve hypoxic condition of tumor microenvironment (TME). As a proof-of-concept study, GIM demonstrates the admirable tumor ablation under NIR irradiation in vivo.
关键词： near-infrared light,metal-organic frameworks,reactive oxygen species,nanozyme,gold nanoparticles
更新于2025-09-23 15:19:57
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Platform for molecular-material dual regulation: A direct Z-scheme MOF/COF heterojunction with enhanced visible-light photocatalytic activity
摘要： Series of novel metal-organic framework/covalent organic framework (MOF/COF) hybrid materials were constructed by encapsulating MOF with highly stable TTB-TTA (a COF synthesized from 4,4',4''-(1,3,5-triazine-2,4,6-triyl)tribenzaldehyde (TTB) and 4,4',4''-(1,3,5-triazine-2,4,6-triyl)trianiline (TTA)) layer, inheriting their merits of high crystallinity, large surface area, outstanding visible-light response and tunable band gaps. The introduction of NH2-MIL-125(Ti) into the hybrid materials could modulate their optical, electronic and redox properties, and promote the charge separation owing to the formation of heterojunction, thus resulting in an enhanced photocatalytic performance for organic pollutant decomposition. As such, NH2-MIL-125(Ti)/TTB-TTA composite has a much higher photodegradation kinetic of methyl orange (MO) which is over 9 and 2 times the rates of pure NH2-MIL-125(Ti) and TTB-TTA, respectively. This versatile molecular-material platform can achieve dual adjusting modes consisting of a COF molecular engineering and a MOF type screening strategy, which will be applicable to a wide range of fields.
关键词： metal-organic frameworks,covalent organic frameworks,heterogeneous photocatalysis,Z-scheme heterojunction,visible-light-driven
更新于2025-09-19 17:15:36
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Thiophene insertion for continuous modulation of the photoelectronic properties of triphenylamine-based metal–organic frameworks for photocatalytic sulfonylation–cyclisation of activated alkenes
摘要： Pharmaceutically meaningful conversions like photocatalytic sulfonylation call for the precise control of the photoelectronic properties of photocatalysts. A ligand engineering strategy of inserting different numbers of thiophenes into the scaffold of triphenylamine (TPA)-based ligands was developed to improve the visible light absorption, enhance the oxidation potentials of the ground states, and decrease the reduction potentials of the excited states, providing a powerful tool for continuous modulation of the photoelectronic properties of metal–organic framework (MOF)-based heterogeneous photocatalysts. The ligand inserted with two thiophenes was found to possess a well-balanced photoelectronic performance, endowing the corresponding MOF Zn–BCTA with good visible light-harvesting ability and a moderate excited-state reduction potential with minimal over-potential for photoinduced generation of sulfonyl radicals while avoiding the competitive over-reduction of the sulfonyl moieties. The breaking of the C3-symmetry of the TPA-based ligand forged a distorted coordination geometry of the Zn4O nodes of the MOF to provide potential active sites to facilitate the fixation and activation of α,β-unsaturated carbonyl substrates, and the two-fold interpenetrated frameworks further enhanced the spatial proximity between the encapsulated substrate and the photoredox-active centre. The synergy of the well-tuned photoelectronic properties of Zn–BCTA and the spatial confinement effect within the pores benefited the tandem sulfonylation–cyclisation of unsaturated alkenes in an efficient and diastereoselective mode for the construction of bio-interesting sulphoyl isoquinolinediones/oxindoles.
关键词： ligand engineering,sulfonylation,cyclisation,metal–organic frameworks,photocatalysis
更新于2025-09-19 17:15:36
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A multifunctional anionic 3D Cd(II)-MOF derived from 2D layers catenation: Organic dyes adsorption, cycloaddition of CO2 with epoxides and luminescence
摘要： An anionic Cd(II)-based metal-organic framework, {[Cd(L)(bpb)0.5(H2O)]·H2O·[(CH3)2NH2]+}n (HL-7, HL is the initial of the author Hui-Ling Liu; H3L = 2′,6′-dimethyl-[1,1′-biphenyl]-3,4′,5-tricarboxylic acid and bpb = 1,4-bis(pyrid-4-yl)benzene), has been hydrothermally synthesized and structurally characterized. Interestingly, HL-7 reveals a three dimensional (3D) frameworks which are constructed from catenation of 2D layers. Further studies prove that as an anionic framework, HL-7 could be a good candidate as adsorption materials for cationic organic dyes, such as methylene blue (MB+) and rhodamine B (RhB+). Moreover, catalytic properties for the cycloaddition of CO2 with epoxides and luminescent property of HL-7 are also investigated at normal temperature and pressure.
关键词： Catalysis,Dye adsorption,Luminescence,Metal-organic frameworks
更新于2025-09-19 17:15:36