Latest ArticlesPhotocatalysis is widely regarded as a highly promising sustainable technique for addressing the challenges posed by environmental pollution and energy provision. In recent years, metal-loaded MOFs has become a rising star within the domain of photocatalysis due to its high specific surface area and porosity, adjustable structure, diverse and abundant catalytic components, which has exhibited excellent photocatalytic activity and exhibit great potential in a range of disciplines. In this paper, the principles for evaluating the photocatalytic performance of MOFs-based materials were firstly introduced, and some typical examples were also listed accordingly. Along with this, particular emphasis is paid to the main factors affecting the photocatalytic performance of metal-loaded MOFs. Then the synthesis and design strategies of MOFs loaded metal entities of varying sizes (single atoms, nanoclusters, and nanoparticles), and their applications in photocatalytic CO2 reduction, hydrogen production, photooxidation and photocatalytic hydrogenation were summarized and discussed. Finally, the opportunities and challenges faced in this kind of MOFs-based composites were analyzed from different perspectives. This report is expected to help researchers design and develop high-performance MOFs-based photocatalytic materials.
An ionic liquid assisted hydrogel modified silica was synthesized using a one-pot polymerization and physical coating technique and subsequently applied to mixed-mode liquid chromatography. Analytical techniques, including Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and elemental analysis, etc., confirmed the successful prepared of this innovative stationary phase. The unique combination of amide, long alkyl chain, and imidazole ring in the hydrogel coating enables the stationary phase to function effectively in hydrophilic/reversed-phase/ion exchange liquid chromatography. Notably, the stationary phase exhibited superior separation performance owing to the synergistic effect of the ionic liquid and hydrogel. This was particularly evident when analyzing various analytes such as organic acids, nucleosides/bases, polycyclic aromatic hydrocarbons (PAHs) and anions. Furthermore, under our operating conditions, an excellent column efficiency of 53, 642.9 plates/m was achieved for theobromine. In summary, we have proposed a straightforward strategy to enhance the separation performance of hydrogel coatings in liquid chromatography, thereby broadening the potential applications of hydrogels in the field of separation.
The rapid development of microfluidic technology has led to the evolution of microdroplets from simple emulsion structures to complex multilayered and multicompartmental configurations. These advancements have endowed microdroplets with the capability to contain multiple compartments that remain isolated from one another, enabling them to carry different molecules of interest. Consequently, researchers can now investigate intricate spatially confined chemical reactions and signal transduction pathways within subcellular organelles. Moreover, modern microdroplets often possess excellent optical transparency, allowing fluorescently labelled, multi-layered, and compartmental droplets to provide detailed insights through real-time, in situ, and dynamic fluorescence imaging. Hence, this review systematically summarizes current methodologies for preparing multicomponent microdroplets and their applications, particularly focusing on fluorescent microdroplets. Additionally, it discusses existing critical challenges and outlines future research directions. By offering a comprehensive overview of the preparation methods and applications of fluorescent microdroplets, this review aims to stimulate the interest of researchers and foster their utilization in more complex and biomimetic environments.
Metal-organic frameworks (MOFs) with superior physicochemical properties have great potential for applications in chromatographic separation. However, currently popular methods for the synthesis of MOF-based silica composite materials usually require the use of harmful organic solvents and long-term high-temperature sealing reactions. In order to respond to the needs of green chromatography, it is urgent to develop a new green organic-solvent-free strategy for the synthesis of MOF@SiO2 composites. MIP-202 is a zirconium-MOF constructed from zirconium ion and l-aspartic acid, which features green synthesis as well as good hydrolytic stability and chemical stability. In this paper, SiO2-NH2 was first prepared in a hydrophilic deep eutectic solvent, and then an amino acid-based MOF material (MIP-202) was modified on the surface of the SiO2-NH2 in an aqueous solution to obtain a MIP-202@SiO2 composite material. The multi-mode separation performance of MIP-202@SiO2 as a promising liquid chromatographic stationary phase was particularly evaluated and the separation mechanisms were discussed. The MIP-202@SiO2 column exhibited excellent separation ability for aromatic positional isomers. In addition, chiral enantiomers and hydrophilic analytes were also satisfactorily detected and separated. This work provides a new approach for the facile synthesis of MOF-based liquid chromatographic separation material by using green deep eutectic solvent and water as the reaction media.
An N-heterocyclic carbene (NHC) catalyzed enantioselective cyclisation and trifluoromethylation of olefins with cinnamaldehydes via radical relay cross-coupling in the presence of Togni reagent is reported and δ-lactones tolerated with stereogenic centers at β- and γ-positions are obtained in moderate to high yields and with high enantioselectivities. Further computational studies explain that the radical cross-coupling step is the key to determining the enantioselectivity. Energy analysis of key transition states and intermediates also provides a reasonable explanation for the difficulty of diastereoselective control. DFT calculations also reveal that the hydrogen-bonding interaction plays a vital role in the promotion of this chemistry.
Immunotherapy offers significant potential but is often hampered by the immunosuppressive environment in oral squamous cell carcinoma (OSCC). To address this, we propose an enhanced immunotherapeutic strategy that revitalizes the tumor immune microenvironment (TIME) in OSCC by integrating upconversion-based photodynamic therapy (PDT) with chemotherapy. Using a red blood cell membrane-inspired biomimetic nanoplatform, our approach concurrently delivers chlorin e6@upconversion nanoparticles (Ce6@UCNP) and doxorubicin (DOX). By leveraging fluorescence resonance energy transfer (FRET) for 980 nm to 660 nm upconversion excitation, we address challenges such as limited tissue penetration and tissue damage, as well as nanoplatform issues including immunogenicity and targeting inaccuracy Our integrated approach enhances PDT and chemotherapy with the goal of transforming immunologically "cold" tumors into "hot" ones through a cascaded therapy, thereby revitalizing the tumor immune microenvironment in OSCC.
The oxygen reduction reaction (ORR) is a crucial process in Zn-air systems, and the catalyst plays a significant role in this reaction. However, reported catalysts often suffer from poor durability and stability during the ORR process. Herein, we synthesized La-Fe bimetallic nanoparticles encapsulated in a N-doped porous carbon dodecahedron (La-Fe/NC) originated from ZIF-8 by a simple direct carbonization. The La-Fe/NC catalyst had a numerous mesopores and dendritic outer layer generated by carbon nanotubes (CNTs), forming a high conductivity network that helped to optimize electron transfer and mass transport in the ORR process. The effect of different doping transition metals and metal ratios on the ORR activity of Zn-air batteries was investigated. In alkaline media, the La-Fe/NC showed the highest ORR catalytic activity, with a half-wave potential (E1/2) of 0.879 V (vs. RHE, Pt/C 0.845 V). After 5000 cycles, the E1/2 of the La-Fe/NC catalyst only decreased by 7 mV, and its performance in stability tests and methanol tolerance tests was superior to Pt/C. When used as the air electrode in a Zn-air battery, the La-Fe/NC catalyst demonstrated an excellent specific capacity of 755 mAh/g and a peak power density of 179.8 mW/cm2. The results provide important insights for the development of high-performance Zn-air batteries and new directions for the design of ORR catalysts.
PBQ [1-(4-chlorophenyl)-3-(pyridin-3-yl)urea], an enormous potent molluscicide, showed excellent Pomacea canaliculata (P. canaliculata) control activity and low toxicity for other aquatic organisms, but its snail-killing mechanisms are still not fully understood. We employed an optical method to elucidate PBQ action via a novel fluorescent viscosity probe, NCV. As the viscosity in the test solutions increased, compared with that in pure ethanol, a 54-fold fluorescence intensity enhancement of NCV was observed in 310 cP of 90% glycerol. Furthermore, NCV successfully exhibited a selective fluorescence response towards monensin-induced cellular viscosity changes in HepG2 cells. The liver, stomach, and foot plantar of the tested snails were frozen and sectioned for fluorescent imaging experiments after the treatment with different PBQ concentrations over various times. A significant fluorescent increase in the snail's liver was observed upon exposure to 0.75 mg/L PBQ for 72 h, which highlighted an increase in viscosity. Hematoxylin and eosin (HE) staining further supported PBQ-induced liver damage with a viscosity increase in P. canaliculata. Our study provides a new rapid optical visualization method to study the killing mechanisms of PBQ and may help discover new chemicals that control snail populations.
Axially chiral binaphthol have achieved great success in asymmetric catalysis. Compared to α-binaphthol, axially chiral aryl-β-naphthol are far less reported. Here, we report a method of asymmetric catalysis to construct β-naphthol with up to 99% yield, 95.5:4.5 enantiomeric ratio, using alkynyl esters as precursors and chiral phosphonic acid (CPA)/Lewis acid as catalysts. Key steps involve oxygen transfer and de novo arene formation to set up the chiral axis. Moreover, this methodology provides a versatile platform for structurally divergent synthesis of atroposelective β-naphthol analogs, which are widely found in bioactive molecules and asymmetric catalysts.
Exploring transition metal sulfide electrocatalysts with high-efficiency for hydrogen evolution reaction (HER) is essential to produce H2 fuel through water splitting. Herein, novel nickel tungsten sulfide heterojunction (NiS-WS2) with a nanowoven ball-like structure were directed synthetized by a facile hydrothermal method. The hierarchical NiS-WS2 exhibited excellent HER activity with a relatively small overpotential of 142 and 137 mV at 10 mA/cm2 in 0.5 mol/L H2SO4 and 1 mol/L KOH, which is much better than that of single NiS and WS2. The impressive performance of NiS-WS2 heterojunction is owed to the collective synergy of special morphological and more exposed active sites between the crystal interfacial of NiS and WS2. In addition, the hierarchical NiS-WS2 can facilitate the transport of charge/mass by optimized electronic structure, which further improves the HER activity of electrocatalysts. These outcomes provide a simple method to prospect towards the design and application of heterostructures as efficient electrocatalysts, shedding some light on the development of functional materials in energy chemistry.
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