Covalent organic frameworks (COFs) are a promising platform for heterogeneous photocatalysis due to their stability and design diversity, but their potential is often restricted by unmanageable targeted excitation and charge transfer. Herein, a bimetallic COF integrating photosensitizers and catalytic sites is designed to facilitate locally ultrafast charge transfer, aiming to improve the photocatalytic reduction of CO. The strategy uses a "one-pot" method to synthesize the bimetallic COF (termed PBCOF) through in situ Schiff-base condensation of Pyrene with MBpy (M = Ru, Re) units.
View Article and Find Full Text PDFCovalent organic frameworks (COFs), with their accessible nanoscale porosity, selectable building blocks, and precisely engineered topology, offer unique benefits in the design of room-temperature phosphorescent (RTP) materials. However, their potential has been limited by phosphorescence quenching caused by interlayer π-π stacking interactions. This paper presents a novel strategy to enhance RTP in heavy-atom-free COFs by employing a donor-acceptor (D-A) system that leverages the Förster resonance energy transfer (FRET) and Dexter energy transfer (DET) mechanisms.
View Article and Find Full Text PDFCO electroreduction (CORR) to generate valuable chemicals in acidic electrolytes can improve the carbon utilization rate in comparison to that under alkaline conditions. However, the thermodynamically more favorable hydrogen evolution reaction under an acidic electrolyte makes the CORR a big challenge. Herein, robust metal phthalocyanine(Pc)-based (M = Ni, Co) conductive metal-covalent organic frameworks (MCOFs) connected by strong metal tetraaza[14]annulene (TAA) linkage, named NiPc-NiTAA and NiPc-CoTAA, are designed and synthesized to apply in the CORR in acidic electrolytes for the first time.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs), characterized by tunable porosity, high surface area, and diverse chemical compositions, offer unique prospects for applications in optoelectronic devices. However, the prevailing research on thin-film devices utilizing MOFs has predominantly focused on aspects such as information storage and photosensitivity, often neglecting the integration of the advantages inherent in both photonics and electronics to enhance optical memory. This work demonstrates a light-mediated resistive memory device based on a highly oriented porphyrin-based MOFs film, in which the resistance state of the memristor is modulated by light, realizing the integration of the perception and storage of optical information.
View Article and Find Full Text PDFElectrochemical reduction of CO to multicarbon (C) products with added value represents a promising strategy for achieving a carbon-neutral economy. Precise manipulation of the catalytic interface is imperative to control the catalytic selectivity, particularly toward C products. In this study, a unique Cu/UIO-Br interface is designed, wherein the Cu(111) plane is co-modified simultaneously by Br and O from UIO-66-Br support.
View Article and Find Full Text PDFThe integration of hydrogen-bonded organic frameworks (HOFs) into electronic devices holds great promise due to their high crystallinity, intrinsic porosity, and easy regeneration. However, despite their potential, the utilization of HOFs in electronic devices remains largely unexplored, primarily due to the challenges associated with fabricating high-quality films. Herein, a controlled synthesis of HOF nanofilms with smooth surface, good crystallinity, and high orientation is achieved using a solution-processed approach.
View Article and Find Full Text PDFHalogenated organic compounds are a kind of common environmental pollutants. Photocatalytic dehalogenation of C-halogen (C-X) bonds to C-H bonds can not only control environmental pollution but also realize important organic conversion reactions. However, the electron transfer kinetics of photocatalytic reduction of the C-X bond for semiconductor/MOF composites has remained unexplored.
View Article and Find Full Text PDFN6-methyladenosine (m A) and alternative polyadenylation (APA) are important regulators of gene expression in eukaryotes. Recently, it was found that m A is closely related to APA. However, the molecular mechanism of this new APA regulation remains elusive.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2020
The metal corrosion possesses a serious threat to the safety and loss of property. The anticorrosion study on metal-organic frameworks (MOFs) remains rarely reported. Therefore, it is desirable to build MOFs-based anticorrosion coating with long-term corrosion resistance.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2018
A novel dual-emitting metal-organic framework based on Zr and Eu, named as UiO-66(Zr&Eu), was built using a clever strategy based on secondary building units. With the use of polymers, the obtained UiO-66(Zr&Eu) was subsequently deposited as thin films that can be utilized as smart thermometers. The UiO-66(Zr&Eu) polymer films can be used for the detection of temperature changes in the range of 237-337 K due to the energy transfer between the lanthanide ions (Eu in clusters) and the luminescent ligands, and the relative sensitivity reaches 4.
View Article and Find Full Text PDFTemperature plays a crucial role in both scientific research and industry. However, traditional temperature sensors, such as liquid-filled thermometers, thermocouples, and transistors, require contact to obtain heat equilibrium between the probe and the samples during the measurement. In addition, traditional temperature sensors have limitations when being used to detect the temperature change of fast-moving samples at smaller scales.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2018
Engineering novel dual-emitting metal-organic frameworks (MOFs) with wide emission ranges for application as ratiometric temperature sensors is still a challenge. In this paper, two novel dual-emitting MOFs with intergrated lanthanide metals and luminescent ligand in a UiO-66-type structure, named Ln@UiO-66-Hybrid, were prepared via the combination of postsynthetic modification and postsynthetic exchange methods. Subsequently, the as-synthesized MOFs were deposited onto fluorine tin oxide substrates through electrophoretic deposition by taking advantage of the charges from the unmodified carboxylic groups of the MOFs.
View Article and Find Full Text PDFUntil now, it has been a challenge to prepare lanthanide metal-organic framework films on traditional substrates, like zinc plate, indium oxide (ITO), and fluorine-doped tin oxide (FTO) glasses in a rapid and facile method. In this paper, continuous and dense Ln-BTC MOFs films on unmodified low-cost substrates have been rapidly and easily fabricated though the newly developed electrophoretic deposition (EPD) method in 5 min. Moreover, the as-prepared luminescent films were successfully used for the detection of nitrobenzene (NB), trinitrotoluene (TNT) in gas phases, as well as NB, Cr ions for detection in solution.
View Article and Find Full Text PDFThe integration of porous metal-organic frameworks onto the surface of materials, for use as functional devices, is currently emerging as a promising approach for gas sensing and flexible displays. However, research focused on potential applications in electronic devices is in its infancy. Here we present a facile strategy by which interpenetrated, crystalline metal-organic framework films are deposited onto conductive metal-plate anodes via in situ temperature-controlled electrochemical assembly.
View Article and Find Full Text PDFOrganic dye pollutants become a big headache due to their toxic nature to the environment, and it should be one of the best solutions if we can separate and reuse them. Here, we report the synthesis and characterization of a microporous anion metal-organic framework (MOF) with Lewis basic sites-rich based on TDPAT (2,4,6-tris(3,5-dicarboxylphenylamino)-1,3,5-triazine) ligand, FJI-C2, which shows high adsorption and separation of cationic dye based on the charge-exclusive effect. Compared to other MOF materials, FJI-C2 shows the largest adsorption amount of methylene blue (1323 mg/g) at room temperature due to the nature of the anion frameworks and high surface area/pore volume.
View Article and Find Full Text PDFElectrochemically-assisted microwave deposition technology, a facile method for the fabrication of luminescent metal-organic framework (LMOF) films, is presented herein. This method was further developed into a versatile method for preparing patterned LMOF films. The strategy based on this method can spatially locate microcrystals of MOFs on a surface, which provides great promise in anti-counterfeiting barcode applications.
View Article and Find Full Text PDFPalladium-pyridyl catalytic films, (PdCl2/bpy)n, were created by alternating immersions of a substrate in PdCl2 and bpy (bpy=4, 4'-bipyridyl) solutions. The as-prepared (PdCl2/bpy)10 catalyst demonstrated a remarkable catalytic activity toward hydrogenation of styrene under mild conditions and the turnover frequency (TOF) is as high as 6944h(-1). Pd(II) ions of (PdCl2/bpy)n films are in situ reduced to Pd nanoparticles (NPs) during the hydrogenation of styrene process, which results in the catalytic activity of the films.
View Article and Find Full Text PDFNew porous metal-organic framework (MOF) films based on the flexible ligand 1,3,5-tris[4-(carboxyphenyl)oxamethyl]-2,4,6-trimethylbenzene (H3TBTC) were fabricated on α-Al2O3 substrates under solvent thermal conditions. The factors affecting the fabrication of films, such as the temperature of pre-activation and the dosage of the reagents, were investigated. Tuning the subtle factors on film fabrications, a series of MOF thin films with different morphologies and grain sizes were prepared.
View Article and Find Full Text PDF(PW(12)-TH)(n) multilayer films (PW(12)=PW(12)O(40)(3-), TH=thionine) were deposited successfully on core-shell structured Fe(3)O(4)@SiO(2) magnetic microspheres through layer-by-layer (LbL) self-assembly method. The physical and photocatalytic properties of such magnetic microspheres coated with (PW(12)-TH)(n) films have been characterized by SEM, FTIR, and UV-vis spectra. The microspheres exhibit better photocatalytic activity toward the degradation of methyl orange (MO) under visible light irradiation than the quartz slides support.
View Article and Find Full Text PDFThree sub-10 nm platinum nanoparticles (PtNPs) with distinctive morphologies were developed by using cucurbit[6]uril (CB[6]) as stabilizing agent and support. Both the size and shape of the PtNPs were simultaneously controlled by tuning the reducing agents. The prepared NPs have been comprehensively characterized by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and cyclic voltammetry.
View Article and Find Full Text PDFAiming at investigating the effect of structure on electrocatalytic properties, Pd(50)Ru(50) nanoparticles (NPs) with three different structures were carefully designed in a one-pot polyol process for application in formic acid electrooxidation. The three structures are: (1) single-phase PdRu nanodendrites (denoted as PR-1), (2) a mixed-phase mixture of PdRu nanodendrites and monometallic Ru NPs (denoted as PR-2), and (3) a mixed-phase mixture of monometallic Pd and Ru NPs (denoted as PR-3). From PR-1 to PR-3, the structure was varied from single-phase to mixed-phase.
View Article and Find Full Text PDFMultilayer films (PW(12)-TH)(n) (PW(12)=PW(12)O(40)(3-), TH=thionine) were immobilized on porous anatase TiO(2) microspheres by layer-by-layer (LbL) self-assembly method. The porous structure of TiO(2) was confirmed by transmission electron microscopy (TEM). Scanning electron microscopy (SEM) showed that TiO(2) template particles had a round shape with an average diameter of 250 nm.
View Article and Find Full Text PDF(TH)(3)PW(12) (TH=thionine, PW(12)=PW(12)O(40)(3-)) composite was prepared by direct precipitation of TH and PW(12). The (TH)(3)PW(12) was characterized via UV-vis spectrum, FT-IR, SEM, and BET surface area. PW(12) was intact during the precipitation process.
View Article and Find Full Text PDFThe dilacunary decatungstogermanate [γ-GeW(10)O(36)](8-) (GeW(10)) and the monolacunary undecatungstogermanate [β(2)-GeW(11)O(39)](8-) (GeW(11)) were employed as polyanions to layer-by-layer self-assembly with cationic thionine (TH) dye. The (GeW(10)/TH)(n) and (GeW(11)/TH)(n) composite films were characterized by UV-vis spectra, atomic force microscopy images (AFMs) and cyclic voltammograms (CV). Their photocatalytic activities were evaluated by photocatalytic degradation of methyl orange aqueous solution under sunlight irradiation.
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