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Creation of Photoactive Inorganic/Organic Interfaces Using Occlusion Electrodeposition Process of Inorganic Nanoparticles During Electropolymerization of 2,2′:5′,2′′-Terthiophene
摘要： Photoactive (IOI) inorganic/organic interface assemblies were prepared using an occlusion electrodeposition method. Poly-2,2′:5′,2′′-Terthiophene (PTTh) were the organic thin films that occluded each of CdS, TiO2, and Zn-doped WO3 nanoparticles. The energy band gap structures were investigated using spectroscopic and electrochemical techniques. The obtained assemblies were investigated in aqueous solutions under both dark and illuminated conditions. The results were compared with the behavior of PTTh thin film. Oxygen played an important role in minimizing electron/hole recombination as was evident by observed very low photocurrent when oxygen was removed by nitrogen purge. Results show that PTTh/CdS gave the greatest photocurrent, followed by PTTh/Zn-WO3 and PTTh/TiO2.
关键词： Occlusion,Interface,Organic semiconductors,Photoelectrochemistry,Inorganic
更新于2025-09-04 15:30:14
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Two bimetallic metal–organic frameworks capable of direct photocatalytic degradation of dyes under visible light
摘要： Two bimetallic metal–organic frameworks (MOFs), specifically {2[LiM(TDA)2(DMF)]·NH2+(CH3)2}n (M = Co (HNU-29) or Zn (HNU-30), TDA = 2,5-thiophenedicarboxylate), were synthesized by solvothermal methods. X-ray crystal structures of the two MOFs showed them to be isostructural. Thus, in both cases, the metal secondary building units were connected by TDA2? ligands to form a 3D framework whose structure can be simplified to the twofold interpenetrated dia net. HNU-29 showed excellent photocatalytic activity for the degradation of methylene blue (MB) under visible light even without the addition of H2O2 as an electron acceptor, remaining stable even after several cycles of reuse. The MB degradation followed first-order kinetics, and the photocatalytic degradation mechanism was found to be related to the effective ligand-to-metal charge transfer within the framework.
关键词： Photocatalysis,Methylene blue,Metal–organic frameworks,Visible light,Dye degradation
更新于2025-09-04 15:30:14
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A Metal‐Organic‐Framework‐Derived g‐C3N4/α‐Fe2O3 Hybrid for Enhanced Visible‐Light‐Driven Photocatalytic
摘要： As one of the most efficient systems for photocatalytic hydrogen evolution, the Z-scheme system consisting of different semiconductors with a reversible donor-acceptor pair has attracted great attention. Considering for the nontoxicity and low cost of photocatalysts, a series of g-C3N4/α-Fe2O3 hybrids were rationally constructed based on the Z-scheme mechanism for the first time using a metal-organic framework template approach that can fine-tune the compositions and properties of the hybrids. An optimized hybrid, g-C3N4/α-Fe2O3-2, exhibited prominent photocatalytic water splitting performance with a visible light response. Under irradiation of visible light (λ > 420 nm), the hybrid shows a high durability and superior hydrogen production rate of 2066.2 μmol g-1 h-1 from water splitting, which is approximately three times greater than that of bulk g-C3N4 because of the effective separation of photo-excited charge carriers by two narrow bandgap semiconductors tightly coupled with the Z-scheme structural feature.
关键词： Z-scheme system,hydrogen evolution,g-C3N4/α-Fe2O3 hybrid,metal-organic frameworks
更新于2025-09-04 15:30:14
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Synthesis and characterization of luminescent metal–organic frameworks for the selective recognition of Cu2+ cation and Tryptophan
摘要： Three metal-organic frameworks (MOFs), namely, [Mn(CPP)2(H2O)]n (I), [Cd(CPP)2(H2O)]n (II) and {[Zn2(CPP)2(CO3)]·(ClO4)·(H2O)2}n (III) (HCPP = 4'-(4-(4-carboxylphenoxy)-2,2':60,20-terpyridine), were successfully achieved under hydrothermal conditions. The as-synthesized coordination polymers have been characterized by IR spectroscopy, elemental analyses and single crystal X-ray diffraction. Single-crystal X-ray diffraction analyses indicate that compounds ⅠⅠ and ⅡⅡ display isomorphous and isostructural, in which the central metal ions present distorted octahedral configurations. ⅠⅠ and ⅡⅡ feature fascinating 3D frameworks based on p/p and CeH/p interactions between the pyridine rings ligands, while compound ⅢⅢ possesses a 3D net interlinked via C-H/p interactions appertaining CPP ligands. In their 3D frameworks, the {MnN3O3}, {CdN3O3} and {ZnO2N3}e{ZnO2N3} building units are observed, respectively. Luminescent properties of coordination polymer ⅡⅡ and ⅢⅢ demonstrate that they may be acted as fluorescent sensors toward Cu2+ cation and Tryptophan, respectively. Furthermore, investigations on magnetic property reveal that coordination polymer ⅠⅠ presents antiferromagnetic coupling.
关键词： Magnetic analysis,Luminescent recognition,Transition metal ions,Hydrothermal synthesis,Metal organic frameworks
更新于2025-09-04 15:30:14
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Highly Selective Fluorescent Probe for Hg2+ and MnO4? by the Two-fold Interpenetrating Metal-organic Framework with Nitro Functionalized Linkers
摘要： A novel nitro functionalized Co(II) based two-fold interpenetrating metal-organic framework (MOF), [Co(NPDC)(bpee)]·DMF·2H2O (1) (NPDC = 2-nitro phenylenedicarboxylate, bpee = 1,2-bis(4-bipyridyl)ethylene) has been synthesized by solvothermal method and structurally characterized. The complex consists of a 3D structure in which the nitro functionalized ligand (NPDC) and bipyridine type linkers (bpee) coordinated to Co(II), leading to a fsc type 3,5-c binodal net. The complex shows fluorescent emission both in solid state and in aqueous solution. What’s more, it exhibits a high selectivity for the sensing of MnO4? and heavy metal ion Hg2+ in water by quenching or enhancing luminous intensity, respectively. Naked eyes can even recognize the changes in fluorescence intensities. This work represents a new approach for design and fabrication of functionalized metal-organic frameworks decorated with the nitro group in pore channels, induced by the pre-modified method. Moreover, the detection of Hg2+ and MnO4? indicates the opportunities of the complex be prominent fluorescent probes in potential applications.
关键词： SBUs,crystal engineering,Metal-organic frameworks,fluorescence
更新于2025-09-04 15:30:14
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Process Analytical Technology for Online Monitoring of Organic Reactions by Mass Spectrometry and UV–Vis Spectroscopy
摘要： Process analytical technologies (PATs) are used in the pharmaceutical and other industries to monitor chemical processes in real-time with analytical instrumentation. Each PAT analyzer brings its own advantages and disadvantages to the process, and multiplexing PAT analyzers can be advantageous as they can provide confirmatory measurements and increase the overall confidence of the analysis. In a pedagogical setting, online reaction monitoring enables the instructor to explain the fundamentals of instrumental techniques while highlighting pertinent real-world applications. Here we present a teaching laboratory exercise in which students monitor an amide bond formation reaction by flow UV?vis spectroscopy and by mass spectrometric analysis. The coupling of these two specific instruments allows students to investigate two instruments in one laboratory exercise, to explore the fundamentals behind each, and to contemplate the advantages and disadvantages of these instrumental methods. The coupling of the two instruments was aided by 3D printing which allowed students to explore how rapid prototyping can enable the development of innovative procedures.
关键词： Organic Chemistry,Mass Spectrometry,UV?Vis Spectroscopy,Laboratory Instruction,Instrumental Methods,Hands-On Learning/Manipulatives,Upper-Division Undergraduate,Analytical Chemistry,Reactions
更新于2025-09-04 15:30:14
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Charge transport layers manage mobility and Carrier density balance in light-emitting layers influencing the operational stability of organic light emitting diodes
摘要： Organic light emitting diodes (OLEDs) consist of several organic layers, including the charge injection layer, charge transport layer, and light emitting layer (EML). Of these layers, the charge transport layer is crucial for ensuring device longevity, but its overall effects on charge transport and corresponding device stability are poorly understood. Herein we report the factors influencing differences in lifetime between two OLEDs with different hole transporting layers (HTLs). Comprehensive electrical analysis of the materials and the devices reveals that the mobility, accumulation, trapping, and the transport path of holes in the EML are totally changed by the HTLs. The charge transport layers affect mobility and carrier density balance in the EML through the modification of the charge transport path and the energetic barrier. This results in a reduction of overbalanced polaron density, which is critical for bond dissociation in excitonic interactions. Consequently, device lifetime is increased sevenfold through modification of the HTL structure without any alteration of the EML. These results imply that the analysis of polaronic transport through impedance spectroscopy is a crucial step in determining the requisite electrical properties for charge transport layers, with a view to maximizing the operational stability of OLEDs.
关键词： charge transport,Organic light-emitting diodes,device stability,impedance spectroscopy
更新于2025-09-04 15:30:14
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Metal–Organic Frameworks for Photocatalysis and Photothermal Catalysis
摘要： To meet the ever-increasing global demand for energy, conversion of solar energy to chemical/thermal energy is very promising. Light-mediated catalysis, including photocatalysis (organic transformations, water splitting, CO2 reduction, etc.) and photothermal catalysis play key roles in solar to chemical/thermal energy conversion via the light?matter interaction. The major challenges in traditional semiconductor photocatalysts include insufficient sunlight utilization, charge carrier recombination, limited exposure of active sites, and particularly the difficulty of understanding the structure?activity relationship. Metal?organic frameworks (MOFs), featuring semiconductor-like behavior, have recently captured broad interest toward photocatalysis and photothermal catalysis because of their well-defined and tailorable porous structures, high surface areas, etc. These advantages are beneficial for rational structural modulation for improved light harvesting and charge separation as well as other effects, greatly helping to address the aforementioned challenges and especially facilitating the establishment of the structure?activity relationship. Therefore, it is increasingly important to summarize this research field and provide in-depth insight into MOF-based photocatalysis and photothermal catalysis to accelerate the future development.
关键词： Charge separation,Photocatalysis,Light harvesting,Solar energy conversion,Photothermal catalysis,Metal?organic frameworks
更新于2025-09-04 15:30:14
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Color-tunable lanthanide metal–organic framework gels
摘要： Fluorescence signi?cantly improves the performance of gels. Various strategies, such as embedment and crosslinking, have been used to integrate extrinsic luminophores into gel systems, but the procedures are usually complex. Herein, for the ?rst time, we report gels with intrinsic and tunable emission color prepared with 5-boronoisophthalic acid (5-bop) and Eu3+, Tb3+, and/or Dy3+ similar to the procedure for the preparation of metal–organic frameworks (MOFs). The single-metal gels exhibit intrinsic trichromatic ?uorescence, due to which full-color emissions are readily obtained by tuning the type and/or ratio of Ln3+ ions to prepare mixed-metal gels. The emission is governed by an antenna e?ect and is thus excited with single-wavelength at 275 nm. The nucleation-growth mechanism reveals that the Ln3+ ions and 5-bop produce separated layers, which then grow anisotropically to form nanoribbons by high coordinated valence of Ln3+ ions and biased carboxyl distribution as well as steric hindrance and hydrogen bonds of the boric acid group in 5-bop. The nanoribbons entangle together to generate chemical-physical hybrid gels. To the best of our knowledge, this is the ?rst example of gels with inherent and tunable emission color. Due to their optical and viscoelastic properties, the gels have numerous potential applications such as tunable emission and multi-target detection.
关键词： metal–organic frameworks,lanthanide,gels,tunable emission,Fluorescence
更新于2025-09-04 15:30:14
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Iono-Fluorochromic Nanoparticles Derived from Octa-Pyrene-Modified Polyhedral Oligomeric Silsesquioxanes (POSS) Organic Frameworks for Fluoride Ion Detection
摘要： Three octa-pyrene modified POSS molecules POSS-(C0-Py)8, POSS-(C1-Py)8 and POSS-(C3-Py)8 were successfully prepared by condensation reactions between pyrene carboxylic acid and amino-substituted POSS in good yields, and they were structurally characterized by various spectroscopic methods. All those three POSS molecules could form stable supramolecular hydrogen-bonded organic framework (HOF) structures via amide linkages. Among of them, POSS-(C1-Py)8 displayed the purest excimer emission due to the efficient stacking of pyrene residues in their HOF structures, which was further developed to a highly efficient green-emissive iono-fluorochromic sensor for F- ion. This ratiometric fluorescence sensor displayed the unique selectivity to the F- ion with a detection limit of lower than 5 × 10-5 M and rapid detection within 10 minutes, and it almost did not respond to anions such as Cl-, Br-, I-, AcO-, NO3-, and HPO42- ions. A comparative experiment using ion chromatography method to measure the concentration of the F- ion was conducted, revealing that our iono-fluorochromic sensor had better selectivity and higher anti-interference ability than the traditional chromatography method particularly in the presence of interfering anions. In contrast to the common F- ion fluorescence sensors, which rely on the turn-on or turn-off of the fluorescence, and other traditional chromatography techniques, this type of F- iono-fluorochromic sensors would make it attractive and convenient for fast and reliable detection of F- ion.
关键词： fluoride ion detection,iono-fluorochromic,hydrogen-bonded organic frameworks,POSS,nanoparticles
更新于2025-09-04 15:30:14