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A dual-shell hierarchical protection strategy combining non-hydrolytic sol-gel derived SnO x coating and mesoporous ZSM-5 encapsulation was proposed to simultaneously boost luminescence efficiency and environmental stability of CsPbBr 3 nanocrystals. • Conformal amorphous SnO x layer uniformly passivates surface defects of CsPbBr 3 , the optimized CsPbBr 3 @SnO x sample achieves a PLQY increase from 64% to 74%, and retains 55% and 47% initial PL intensity after 120 min immersion in water and ethanol, respectively. • Secondary encapsulation within hierarchical micro-mesoporous ZSM-5 further reinforces structural robustness, raising the maximum PLQY of CsPbBr 3 @SnO x @ZSM-5 composite up to 76%. The composite exhibits negligible emission shift after 120 min treatment in water, ethanol and tetrahydrofuran, with outstanding retention of luminescence signal. • White light-emitting diode (WLED) assembled with CsPbBr 3 @SnO x @ZSM-5 green phosphor and commercial red K 2 SiF 6 :Mn 4+ phosphor delivers balanced white emission with CIE coordinates of (0.310, 0.307), a color rendering index of 70, correlated color temperature of 6651 K and luminous efficiency of 26.76 lm W −1 , demonstrating great potential for solid-state lighting applications. All-inorganic CsPbBr 3 perovskite nanocrystals (NCs) exhibit excellent optoelectronic properties but suffer from severe instability against moisture, oxygen, heat, and polar solvents due to their ionic lattice, surface defects, and labile ligands, leading to rapid ion migration and photoluminescence quenching. In this work, a dual-shell engineering strategy based on a non-hydrolytic sol-gel (NHSG) route was developed to construct CsPbBr 3 @SnO x and CsPbBr 3 @SnO x @ZSM-5 composite nanostructures. An SnO x -rich interfacial layer was formed on the CsPbBr 3 NCs and subsequently coupled with hierarchical ZSM-5 confinement, contributing to surface-defect passivation and stabilization of the interfacial chemical environment while preserving the perovskite crystal structure and emissive centers. At an optimized Sn/Pb molar ratio of 0.5, the photoluminescence quantum yield (PLQY) increased from 64% to 74%, and an optimal reaction time of 10 min yielded the highest emission efficiency (PLQY≈70%). Moreover, the SnO x coating significantly enhanced environmental stability, with CsPbBr 3 @SnO x retaining 55% and 47% of its initial PL intensity after 120 min exposure to water and ethanol, respectively. Subsequently, hierarchical encapsulation within mesoporous ZSM-5 further reinforced structural robustness and optical stability. The resulting CsPbBr 3 @SnO x @ZSM-5 composite achieved an enhanced PLQY of 76% and exhibited negligible emission shift after immersion in water, ethanol, and tetrahydrofuran for 120 min. In addition, the composite demonstrated excellent stability under continuous UV irradiation, thermal treatment, and ambient storage conditions. Finally, a white light-emitting diode (WLED) device fabricated using CsPbBr 3 @SnO x @ZSM-5 delivered stable white emission with Commission Internationale de l'Éclairage (CIE) coordinates of (0.310, 0.307), a color rendering index (CRI) of 70, a correlated color temperature (CCT) of 6651 K, and a luminous efficiency of 26.76 lm W −1 . These results highlight the effectiveness of the dual encapsulation strategy in simultaneously enhancing the photoluminescence performance and environmental stability of perovskite nanocrystals, providing a viable route toward high-performance optoelectronic and solid-state lighting applications. Download: Download high-res image (303KB) Download: Download full-size image
Pillar[5]arene complexes of the naturally occurring compound bisdemethoxycurcumin (BDMC) were acquired for improving the water solubility and stability of BDMC. As a family member of curcuminoid compounds, BDMC has many interesting therapeutic properties. However, its low aqueous solubility and stability resulted in poor availability and restricted the clinical efficacy. Pillar[5]arenes with hydrophilic ends and a hydrophobic cavity could include with BDMC based on size matching. The synthesized hydrazide-pillar[5]arene (HP5A) and BDMC had a strong host–guest interaction with a 1:1 binding stoichiometry. Furthermore, the HP5A ⊃ BDMC complex could self-assemble into well-defined fibers in water/ethanol solution. This supramolecular complex worked well in vitro for inhibiting the proliferation of hepatoma carcinoma cells HepG2. Remarkably, this method of complexation with pillar[5]arenes visibly reduced the undesirable side effects on normal cells without weakening the anti-cancer activity of the drugs. We expected that the obtained host–guest complex and fibrous assembly would provide a promising platform for delivering drugs with low water solubility.
Background: Keloid is a skin fibroproliferative disease with unknown pathogenesis. Metabolomics provides a new perspective for revealing biomarkers related to metabolites and their metabolic mechanisms.Method: Metabolomics and transcriptomics were used for data analysis. Quality control of the data was performed to standardize the data. Principal component analysis (PCA), PLS-DA, OPLS-DA, univariate analysis, CIBERSORT, neural network model, and machine learning correlation analysis were used to calculate differential metabolites. The molecular mechanisms of characteristic metabolites and differentially expressed genes were identified through enrichment analysis and topological analysis.Result: Compared with normal tissue, lipids have a tendency to decrease in keloids, while peptides have a tendency to increase in keloids. Significantly different metabolites between the two groups were identified by random forest analysis, including 1-methylnicotinamide, 4-hydroxyproline, 5-hydroxylysine, and l-prolinamide. The metabolic pathways which play important roles in the pathogenesis of keloids included arachidonic acid metabolism and d-arginine and d-ornithine metabolism. Metabolomic profiling reveals that 5-hydroxylysine and 1-methylnicotinamide are metabolic indicators of keloid severity. The high-risk early warning index for 5-hydroxylysine is 4 × 108-6.3×108 (p = 0.0008), and the high-risk predictive index for 1-methylnicotinamide is 0.95 × 107-1.6×107 (p = 0.0022).Conclusion: This study was the first to reveal the metabolome profile and transcriptome of keloids. Differential metabolites and metabolic pathways were calculated by machine learning. Metabolomic profiling reveals that 5-hydroxylysine and 1-methylnicotinamide may be metabolic indicators of keloid severity.
Cancer targeted therapies have attracted considerable attention over the past year. Recently, 5-fluouracil (5-FU), which has high toxicity to normal cells and short half-life associated with rapid metabolism, is one of the most commonly used therapies in the treatment of cancer. In this study the folic acid-conjugated pegylated nanoliposomes were synthesized and then loaded into them with 5-FU to improve the anti-tumor efficacy. The average size of liposomes (LPs) was about 52.7 nm which was identified by TEM. In the liposome uptake studies, the level uptake of folate-conjugated liposomes has increased compared to non-conjugated LPs according to LPs concentration, incubation time and presence of concentration of free folic acid (FA). The MTT assay and apoptotic test were carried out in HCT116 and MCF-7 cells for 24 or 48 h. The results revealed that the folate-PEG modified 5-Fu loaded nanoliposomes had strong cytotoxicity to cancer cell compared to pure 5-FU or PEG modified 5-FU loaded liposomes in a concentration- and time-dependent manner, and mainly enhanced the cancer cell death through folate-mediated endocytosis. Hence, the folate-PEG modified nanoliposome is a potential targeted drug-delivery system for the treatment of FR-positive cancers.
5-hydroxymethylfurfural (HMF) obtained from biomass is an important platform chemical for the next generation of plastics and biofuel production. Although industrialized, the high yield of HMF in aqueous systems was rarely achieved. The main problem is that HMF tends to form byproducts when co-adsorbed with water at acid sites. In this study, the pressure was reduced to improve the maximum yield of HMF from 9.3 to 35.2% (at 190 °C in 60 min) in a glucose aqueous solution. The mechanism here involved water boiling as caused by pressure reduction, which in turn promoted the desorption of HMF from the solid catalyst, thereby inhibiting the side reaction of HMF. Furthermore, the solid catalysts could be reused three times without a significant loss of their catalytic activity. Overall, this work provides an effective strategy to improve the yield of HMF in water over heterogeneous catalysts in practice.Keywords:glucose;5-hydroxylmethyfurfural;aqueous phase;heterogeneous catalysts;pressure reduction
A novel fluorescence sensor for successive detection of Cu2+ and Fe3+ based on anti-B18H22 derivative which possesses 5-hydroxyisoquinoline as an ionophore was synthesized via a one-pot and its structure and photophysical properties were characterized by NMR, HRMS, FTIR, UV–vis, PL and theoretical calculation. The fluorophore displays two emission peaks at 460 nm and 670 nm in THF solution coming from the emission of the locally excited state and intramolecular charge transfer fluorescence, respectively. The complex exhibited obvious aggregation-induced emission enhancement (AIEE) characteristics in THF/H2O solution by increasing the aqueous concentration from 70% to 95%. The AIEE molecules showed a high selectivity towards Cu2+ over other metal ions by forming a 2:1 metal-to-ligand complex in THF/H2O (fw = 20%) solution, the fluorescence intensity increased as a linear function of the Cu2+ concentration at 460 nm due to the inhibition of PET effect. The fluorescent emission was quenched linearly by the addition of Fe3+, which provides a method for successive determination of Cu2+ and Fe3+ based on 'off-on-off' fluorescence of the fluorescent. The detection limit of Cu2+ and Fe3+ was 5.7 × 10−6 M and 7.2 × 10−5 M respectively. Morever, a rapid identification of Cu2+ in the aqueous solution by naked eyes can be realized. In addition, the molecules were pH-sensitive, the fluorescence quenching can be observed in strongly alkaline environment. The method has been applied to the determination of copper ions in water samples with satisfactory results.
In this work, HZSM-5, Al-SBA-15 and Al-SBA-15/HZSM-5 were adopted as supporting materials for the nickel-based catalysts used in hydrodeoxygenation process. Incipient wetness impregnation method was employed to load nickel species onto these materials. The physicochemical characterization was carried out using advanced instruments. The effect of composition of nickel-based catalysts on hydrodeoxygenation (HDO) reaction was studied. Support materials of nickel-based catalyst have a significantly impact on HDO activity. The highest selectivity (67.9%) of propyl-cyclohexane was obtained over nickel based Al-SBA-15/HZSM-5 catalyst, and nearly all the eugenol was completely hydrodeoxygenated after reaction. The impact of light fractions existed in bio-oil on phenols upgrading process was investigated. The conversion of eugenol mixed with light fractions reached nearly 100% for all the reactions. Eugenol mixed with light fractions as reactant could reduce ring break reaction during hydrodeoxygenation process. The selectivity of alkanes remained nearly unchanged after adding ethylene glycol into the reactant. However, the selectivity of propyl-cyclohexane was significantly decreased by mixing furfural or acetic acid with eugenol as reactant.
Graphical Low loading : With a small catalyst loading of metal-free and selective ionic liquids (0.1 % based on 2,5-furandicarboxylic acid), bioderived poly(ethylene 2,5-furandicarboxylate) is efficiently prepared with high molecular weight by the electrophilic activation induced by hydrogen bonds, which are formed between the ionic liquid [C 2 MIM] + and the carbonyl oxygen. Green synthesis of bioderived high-molecular-weight poly(ethylene 2,5-furandicarboxylate) (PEF) over metal-free catalysts is a significant challenge. This study focuses on PEF prepared from ethylene glycol and 2,5-furandicarboxylic acid (FDCA) through a direct esterification method with ecofriendly metal-free ionic liquids (ILs) as catalysts. The catalytic activities of a series of imidazolium cations in the presence of various anions are systematically investigated and found to be mainly governed by the anions. Among the ILs studied, 1-ethyl-3-methylimidazolium tetrafluoroborate ([C 2 MIM]BF 4 ) is identified as the best catalyst, showing excellent catalytic activity, selectivity, and stability, even at low catalyst loadings (0.1 mol % w.r.t. FDCA). Optimization of the polymerization parameters enables [C 2 MIM]BF 4 -catalyzed production of PEF with a high number-average molecular weight ( M n =5.25×10 4 g mol −1 ). The relationship between Brønsted acidity and catalytic activity is also investigated and the results show that the trend in catalytic activity is in good agreement with that in Brønsted acidity, as determined by the Hammett method. Additionally, on the basis of experimental results and density functional theory calculations, an electrophilic activation mechanism induced by hydrogen bonds is proposed. This strategy of adjustable acidity and anion structure in ILs provides an opportunity to develop other ILs for bio-based polyesters through green synthesis pathways.
The present report pertains to the synthesis and characterization of six complexes, [Zn2(μ-dmpz)2(Hdmpz)2(H2O)2](ClO4)2 (1) (Hdmpz = 3,5-dimethylpyrazole, dmpz = 3,5-dimethylpyrazolate), Cd(Hdmpz)(L1)2 (2) (L1 = 2-methylbenzoate), [Zn2(μ-dmpz)2(Hdmpz)2(L2)2] (3) (L2 = 3-chlorobenzoate), Zn(Hdmpz)2(L3)2 (4) (L3 = 3,4-dichlorobenzoate), Cd(Hdmpz)4(L4)2 (5) (L4 = 5-bromosalicylate), and Zn2(Hdmpz)4(L5)2·3H2O (6) (L5 = fumarate). These complexes were characterized by EA, IR, SCXRD analysis, and TGA.The X-ray studies show that these complexes have mononuclear to dinuclear structures with tetrahedral/octahedral arrangement around each Zn2+/Cd2+. The Hdmpzs in 2 and 4–6 are monodentate ligated via its neutral N, while 1 and 3 have neutral Hdmpzs and the ionic dmpzs. The CO2− of 3–6 is only monodentate. Compound 2 has both monodentate bridging and chelating bidentate CO2-.Intramolecular N–H···O H-bond from Hdmpz and ClO4- was present in 1. The coordinated O of CO2- in 2 accepts an intramolecular N–H···O H-bond from N-H of the Hdmpz and uncoordinated O of the CO2- in 3, 4 and 5 has an intramolecular N–H···O H-bond with N-H of the Hdmpz. Compound 6 has intramolecular N–H···O H-bonds from the Hdmpz, the uncoordinated O and H2O. The intricate intra- and intermolecular classical H-bonds, Br···O, CH···Cl, CH3···Cl, CH···Br, C–H···O, CH3···O, C···π, O···π, O···C, Cl-π, C–H···π and CH3···π associations are elucidated by X-ray crystallographic studies, which convert discrete units into high-dimensional ordered supramolecular structures.
A hydrostable anionic porous drug carrier MOF with a bcu topology constructed from trinuclear clusters, [(Me2NH2)2Zn3(fdc)4]n·DMA (1) (fdc = 2,5-furandicarboxylate, DMA = dimethylacetamide), was synthesized and structurally characterized. TGA, PXRD, and water vapor sorption results show high thermal and water stability for the framework. 1 exhibits a 3D framework with rectangular channels of 10.0 × 7.7 and 6.1 × 7.8 Å2 along the b axis. Desolvated 1 adsorbs around 17.2 wt% 5-fluorouracil and the cumulative release value of 5-fluorouracil at 72 h was about 93.3% in PBS (pH 7.4) at 37 °C. Results of in vivo zebrafish toxicity tests and in vitro MTT assays of 1 at different concentrations reveal that 1 is nontoxic.
Dielectric materials with high energy density ( U e ) and breakdown strength ( E b ) have played crucial roles in electronic power system and national defense weapons. However, current dielectric materials exhibit low energy storage performance, which restricts the miniaturization and lightweight of electronic devices. Herein, a novel strategy toward synchronously achieving high U e and E b of dielectric materials is designed by introducing low-loading poly(1,5-anthraquinone) (P15AQ) into poly(vinylidene fluoride) (PVDF). The dielectric constant ( ε r ) match between P15AQ and PVDF promotes the uniform distribution of electric field and prevents the early breakdown damage. Meanwhile, introducing P15AQ into PVDF film improves the mechanical properties and decreases the leakage current density. As a result, U e and E b of the composite film reach up to 11.0 J cm − 3 and 559 MV m − 1 , respectively. This work demonstrates that PVDF/P15AQ composites with remarkable comprehensive performance have the potential to achieve wider application in dielectric fields.
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