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- Hanyang University
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Aging of a Vanadium Precursor Solution: Influencing Material Properties and Photoelectrochemical Water Oxidation Performance of Solution-Processed BiVO <sub/>4</sub> Photoanodes
摘要： Metal–organic decomposition is an easy way to fabricate BiVO4 (BVO) photoanodes; however, it often experiences a reproducibility issue. Here, the aging duration of a vanadium precursor solution, vanadyl acetylacetonate in methanol, is identified as a factor that profoundly affects reproducibility. Substantial changes in structural, optical, and electrical properties of BVO films are observed upon varying aging time of vanadium precursor solutions, which subsequently impacts photoelectrochemical (PEC) water oxidation and sulfite oxidation reactions. With the optimum number of aging days (3 d), some deficiency of oxygen is observed, which is accompanied by an increase in carrier concentration and a reduced charge transfer resistance in the PEC device, which produces the highest PEC performance that is comparable to the state-of-the-art undoped BVO photoanodes. The findings point to the importance of understanding solution chemistry and demonstrate that utilization of the understanding of fine adjustment of the composition of BVO films can produce highly reproducible and efficient BiVO4 photoanodes.
关键词： solution aging,metal–organic decomposition,bismuth vanadate,chemical composition,photoelectrochemical water splitting
更新于2025-09-23 15:23:52
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Sustainable Liquid Luminescent Solar Concentrators
摘要： Luminescent solar concentrators (LSCs) are photovoltaic (PV) complementary devices to overcome the mismatch between the Si-based PV cells, response and the solar spectrum, allowing PV urban integration. Challenges for the luminescent layer include the use of abundant and sustainable natural organic molecules. Here, LSCs composed of a glass container and based on bundles of cylindrical hollow-core plastic optical fibers filled with aqueous solutions of R-phycoerythrin (R-PE), extracted from Gracilaria sp. algae are presented. The R-PE solutions absorb in the UV/visible spectral range (300–550 nm) and convert this radiation into red-emission (550–700 nm) with a maximum absolute quantum yield of ≈0.39. In this work, LSCs with distinct geometries are reported, in which the R-PE emission yields optical conversion efficiency values up to ≈6.88% and ≈4.74% for a planar device and for a bundle of cylindrical LSCs, respectively, which are the largest values known for liquid-based LCSs using sustainable emitting centres. Moreover, the coupling of the LSCs to commercial Si-based PV devices yields power conversion efficiency values of ≈0.27% (planar) and ≈23.03 × 10?3%, (bundle). These values illustrate the potential of this approach for the development of natural-based LSCs meeting the requirements of reliable, sustainable, and competitive energy systems.
关键词： sustainability,organic–inorganic hybrids,luminescent solar concentrators,R-phycoerythrin,natural optically active center,bundles
更新于2025-09-23 15:23:52
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Universal Reservior of UV, WL and NIR Light for Long Persistent Luminescence from a Metal-Organic Supramolecular Box
摘要： Long persistent luminescence (LPL) materials have unique photophysical mechanism to store light radiation energy for subsequent release. However, in comparison to the common UV source, white-light (WL) and near-infrared (NIR) excited LPL is scarce. Here we report a metal-organic supramolecular box based on a D-π-A type ligand. Due to the integrated one-photon absorption (OPA) and two-photon absorption (TPA) attributes of the ligand, heavy atom effect of the metal-center, as well as π-stacking and J-aggregation states in the supramolecular assembly, LPL can be triggered by all wavebands from UV, WL to NIR region for the first time. This novel designed supramolecular kit to afford LPL via both OPA and TPA pathways provides potential applications in anti-counterfeiting, camouflaging, decorating, displaying, and so on.
关键词： white light,LPL,TPA,metal-organic box,NIR
更新于2025-09-23 15:23:52
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A New Biscarbazole-Based Metal-Organic Framework for Efficient Host-Guest Energy Transfer
摘要： A new metal–organic framework (MOF), [Zn6L4(Me2NH2+)4·3 H2O] (1) was constructed based on [9,9’-biscarbazole]-3,3’,6,6’-tetracarboxylic acid (H4L) and Zn2+ ions. The porous framework and intense blue fluorescence of the MOF based on the biscarbazole moiety of the ligand could facilitate efficient host to guest energy transfer, which makes it an ideal platform for the tuning of luminescence.
关键词： in situ encapsulation,metal–organic frameworks,energy transfer,host–guest systems,fluorescence
更新于2025-09-23 15:23:52
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Spatially Uniform Shallow Trap Distribution in an Ultrathin Organic Transistor
摘要： In organic electronic materials, charge carrier transport is often limited by disorder-induced trap states very close in energy to the ideal band transport states. We directly view the location and impact of these 'shallow' traps on an ultrathin transistor active layer using Kelvin Probe Force Microscopy. As the transistor turns on, dramatic fluctuations in the surface potential of the active channel suddenly arise due to charge trapping and release processes. Importantly, the spatial distribution of rapid fluctuations in surface potential is uniform throughout the active channel. These facts strongly constrain the microscopic origin of shallow charge traps, and associated efforts to optimize the mobility and noise performance baseline in device applications.
关键词： disorder,charge traps,electrical noise,organic electronics
更新于2025-09-23 15:23:52
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Versatile and Switchable Responsive Properties of a Lanthanide-Viologen Metal-Organic Framework
摘要： Metal–organic frameworks (MOFs) provide intriguing platforms for the design of responsive materials. It is challenging to mobilize as many components as possible of a MOF to collaboratively accomplish multiple responsive properties. Here, reversible photochromism, piezochromism, hydrochromism, ionochromism, and luminescence modulation of an ionic Eu(III) MOF is reported furnished by cationic electron-deficient viologen units and exchangeable guest anions. Mechanistically, the extraordinarily versatile responsive properties are owed to electron transfer (ET), charge transfer (CT), and energy transfer, involving viologen as electron acceptor, anion as electron donor, luminescing Eu(III) as energy donor, and anion-viologen CT complex or ET-generated radical as energy acceptor (luminescence quencher). Moreover, guest anions and waters provide flexible handles to control the ET-based responsive properties. Water release/reuptake or exchange with organic solvents can switch on/off the response to light, while reversible anion exchange can disenable or awaken the responses to pressure, light, and water release/reuptake. The impacts of water and anions on ET are justified by the high polarity and hydrogen-bonding capability of water, the different electron donor strength of anions, and the strong I?-viologen CT interactions. The rich responsive behaviors have great implications for applications such as pressure sensors, iodide detection, and chemical logic gates.
关键词： metal–organic frameworks,electron transfer,charge transfer,luminescence switches,piezochromism
更新于2025-09-23 15:23:52
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A new asymmetric anthracene derivative with high mobility
摘要： An asymmetric anthracene derivative (4-HDPA) was designed and synthesized. With the optimization of proper scenario of fabrication process, top-contact thin film devices based on 4-HDPA exhibit mobility as high as 3.59 cm2 V–1 s–1, while its single-crystal devices exhibit mobility as high as 5.12 cm2 V–1 s–1, which is higher than the symmetrical counterpart of 4-HDPA in both single-crystal and thin film devices.
关键词： organic field-effect transistor (OFET),mobility,asymmetric,anthracene derivative
更新于2025-09-23 15:23:52
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Facile fabrication of cross-linked fluorescent organic nanoparticles with aggregation-induced emission characteristic via the thiol-ene click reaction and their potential for biological imaging
摘要： Over the past several years, the biomedical applications of fluorescent organic nanoparticles (FONs) with aggregation-induced emission (AIE) feature have been extensively explored because the AIE-active FONs could effectively overcome the aggregation caused quenching (ACQ) effect of FONs based on conventional organic dyes. The development of novel methods for synthesis of AIE-active FONs plays a centre role for their biomedical applications. In this work, we reported a facile one-step thiol-ene click reaction for fabrication of AIE-active FONs through conjugation of acrylated PEG and AIE-active tetraphenylethylene (TPE) with two ene bonds using pentaerythritol tetra(3-mercaptopropionate) as the linkage. The successful synthesis of TPE containing AIE-active copolymers was evidenced by various characterization techniques. The particle size and fluorescence properties of the resultant TPE-S-PEG copolymers were evaluated by transmission electronic microscopy and fluorescence spectroscopy. Moreover, the cell viability and cell uptake behavior was also examined to evaluate their potential for biological imaging. We demonstrated that the cross-linked TPE-S-PEG show small size, high water dispersibility, low cytotoxicity and strong fluorescence for tracing. All of these advantages endow the TPE-S-PEG FONs great potential for biological imaging applications. Furthermore, this novel click reaction can take place under mild experimental conditions with high efficiency. It could be also further expanded for preparation of multifunctional AIE-active materials due to the universality of the thiol-ene click reaction and good precursor applicapability. Taken together, we have developed a novel and effective thiol-ene click reaction to fabricate the cross-linked AIE-active FONs, which display excellent physicochemical and biological properties and are promising for biomedical applications.
关键词： thiol-ene click reaction,Aggregation-induced emission,biomedical applications,fluorescent organic nanoparticles,cross-linked FONs
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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Organic Transistor Based on Cyclopentadithiophene-Benzothiadiazole Donor-Acceptor Copolymer for the Detection and Discrimination between Multiple Structural Isomers
摘要： Distinguishing structural isomers is a critical and challenging task for biotechnology, chemical industry, and environmental monitoring. Approaches currently available are limited in terms of selectivity and simplicity. In this paper, a highly sensitive organic field-effect transistor (OFET) using the cyclopentadithiophene-benzothiadiazole (CDT-BTZ) copolymers as a semiconductor is presented for easy and selective detection of different families of structural isomers, as well as between different isomers within each family. High accuracy discrimination is achieved over a range of concentrations using only a single sensing parameter derived from the OFET characteristic transfer curve. As a reference, other homopolymer- and donor–acceptor copolymer-based OFET sensors are examined but do not have an equivalent sensing performance to that of the CDT-BTZ-based OFETs. Investigating the link between isomer absorption and swelling, supramolecular order and energy levels of the active layer reveals a unique effect of each isomer on the energy bands of the semiconducting polymer.
关键词： isomers,donor–acceptor copolymers,gas sensor,organic field-effect transistor,xylenes
更新于2025-09-23 15:23:52