Latest ArticlesHyperterpenoid A (1) and B (2), two pairs of enantiomers, with an unprecedented 6/6/4/6/6 polycyclic skeleton, along with one known compoud hypermonone A (3) were isolated from Hypericum beanii. The racemate (±)-1 and (±)-2 were successfully separated into the two optically pure enantiomers (ee ≥ 99%) using a preparative HPLC system. Their absolute configurations were elucidated by extensive spectroscopic analyses and single-crystal X-ray diffraction method. The related plausible biogenetic pathways were presented. Compound 1-3 showed significant neuroprotective activity and potential anti-inflammatory activity. The result that (+)-2 and (-)-2 presented different anti-inflammatory properties, may lead us to new discovery of structure activity relationship between racemates, enantiomers, and diastereomers, as well as further research regarding the binding of drugs to target proteins.
Exorbitant aldosterone is closely associated with various severe diseases, including congestive heart failure and chronic kidney disease. As aldosterone synthase is the pivotal enzyme in aldosterone biosynthesis, its inhibition constitutes a promising treatment for these diseases. Via a structure-based approach, a series of pyridyl substituted 3,4-dihydrobenzo[f][1,4]oxazepin-5(2H)-ones were designed as inhibitors of aldosterone synthase. Six compounds (5j, 5l, 5m 5w, 5x and 5y) distinguished themselves with potent inhibition (IC50 < 100 nmol/L) and high selectivity over homogenous 11β-hydroxylase. As the most promising compound, 5x exhibited an IC50 of 12 nmol/L and an excellent selectivity factor (SF) of 157, which are both superior to those of the reference fadrazole (IC50=21 nmol/L, SF=7). Importantly, 5x showed no inhibition against steroidogenic CYP17, CYP19 and a panel of hepatic CYP enzymes indicating an outstanding safety profile. As it manifested satisfactory pharmacokinetic properties in rats, compound 5x was considered as a drug candidate for further development.
The power conversion efficiencies (PCEs) of organic solar cells (OSCs) have reached 18% recently, which have already met the demand of practical application. However, these outstanding results were generally achieved with donor-acceptor (D-A) type copolymer donors, which can hardly fulfill the low-cost large-scale production due to their complicated synthesis processes. Therefore, developing polymer donors with simple chemical structures is urgent for realizing low-cost OSCs. Polythiophene (PT) derivatives are currently regarded as promising candidates for such kind of donor materials, which has been illustrated in many works. In this work, two new alkylthio substituted PT derivatives, P301 and P302, were synthesized and tested as donors in the OSCs using Y5 as the acceptor. In comparison, the introduction of fluorine atoms on the backbone of P302 can not only downshift the energy levels, but also greatly improve the phase separation morphologies of the active layers, which is ascribed to the enhanced aggregation effect and the reduced miscibility with the non-fullerene acceptor. As a result, the P302:Y5-based OSC exhibits a significantly improved PCE of 9.65% than that of P301:Y5-based one, indicating the important role of fluorination in the construction of efficient PT derivative donors.
Hematite (α-Fe2O3) is a promising photoanode for photoelectrochemical (PEC) water splitting. However, the severe charge recombination and sluggish water oxidation kinetics extremely limit its use in photohydrogen conversion. Herein, a co-activation strategy is proposed, namely through phosphorus (P) doping and the loading of CoAl-layered double hydroxides (CoAl-LDHs) cocatalysts. Unexpectedly, the integrated system, CoAl-LDHs/P-Fe2O3 photoanode, exhibits an outstanding photocurrent density of 1.56 mA/cm2 at 1.23 V (vs. reversible hydrogen electrode, RHE), under AM 1.5 G, which is 2.6 times of pure α-Fe2O3. Systematic studies reveal that the remarkable PEC performance is attributed to accelerated surface OER kinetics and enhanced carrier separation efficiency. This work provides a feasible strategy to enhance the PEC performance of hematite photoanodes.
This study was to investigate the optimal additions of the cellulose decomposition reaction to obtain the most yield of 5-HMF and other furan derivatives in various biphasic systems with FeCl3-CuCl2 mixed catalysts, and explore its depolymerization kinetics. A series of controllable reactions have been performed under mild environmentally friendly atmosphere. The experiment results showed that 49.13 wt% of 5-HMF was the maximum production along with 2.98 wt% other furan derivatives catalyzed by mixed Lewis acid FeCl3-CuCl2 under the two phases which included high concentration NaCl aqueous phase and n-butanol organic phase at 190 ℃ for 45 min. The conclusion suggested that two-phase systems benefited the yield of 5-HMF, furan derivatives via extracting the target products from reaction phase to organic phase to avoid rehydration of 5-HMF. The kinetic calculation revealed the conversion with mixed catalysts had lower reaction apparent activation energy (21.65 kJ/mol, 190-230 ℃) and the reaction rate was faster than that with acid-based catalysts. Based on experiment exploration, the probable mechanism of cellulose decomposition with FeCl3-CuCl2 was proposed.
Developing an excellent photocatalysis system to remove pesticides from water is an urgent problem in current environment purification field. Herein, a Z-scheme WO3/g-C3N4 photocatalyst was prepared by a facile in-situ calcination method, and the photocatalytic activity was investigated for degradation of nitenpyram (NTP) under visible light. The optimal Z-scheme WO3/g-C3N4 photocatalyst displayed the highest rate constant (0.036 min−1), which is about 1.7 and 25 times higher than that of pure g-C3N4 and WO3, respectively. The improvement of photocatalytic performance is attributed to fast transfer of photogenerated carriers in the Z-scheme structure, which are testified by electron spin resonance (ESR) experiments, photocurrent and electrochemical impedance spectra (EIS) measurements. Moreover, the effects of typical water environmental factors on the degradation NTP were systematically studied. And the possible degradation pathways of NTP were deduced by the intermediates detected by high-performance liquid chromatography-mass spectrometry (HPLC-MS). This work will not only contribute to understand the degradation mechanism of pesticides in real water environmental condition, but also promote the development of new technologies for pesticide pollution control as well as environmental remediation.
Highly active and low-cost catalytic electrodes for urea oxidation reaction (UOR) are always crucial for exploration of urea fuel cells. Herein, novel york-shell-structural Ni2P/C nanosphere hybrids (Ni2P/C-YS) are rationally constructed via a hydrothermal method and subsequent phosphidation treatment under different temperature ranging from 250 ℃ to 450 ℃ for UOR applications. In the in-situ constructed hollow york-shell structure, the coupling of conductive carbon materials and active Ni2P allows numerous interfaces facilitating the electron transfer and thereby accelerating the catalytic kinetics. The results demonstrate that Ni2P/C-YS-350 nanocomposite can boost the UOR process with a low potential of 1.366 V vs. RHE at a current density of 50 mA/cm2 in alkaline electrolyte and afford the superior durability with negligible potential decay after 23 h. This study presents that the carbon coated Ni2P hybrid with the optimized crystallinities and hollow york-shell configurations can be a promising candidate for application in urea fuel cells.
Chinese herbal medicines (CHMs) play an increasingly important role in the field of medicine and affects public health in the world. Although more and more strict has been employed to ensure the quality and safety of CHMs, pesticide residues in CHMs remain a serious issue and are the bottleneck for the global development of CHMs. In this work, we applied molecularly imprinted membrane electrospray mass spectrometry (MIM-ESI MS) for rapid detecting 4 classes of pesticide residues in CHMs, including organophosphorus (OPP), carbamates, pyrethroids and neonicotinoids in CHMs. Compared with our previous ambient ionization method MESI, MIM-ESI is capable of achieving a ~50-fold increase in the detection limit of conventional analytical methods owing to the specificity recognition and unique enrichment of MIM. The optimal experimental conditions were determined, and the method was further validated for its sensitivity and specificity. Our data showed that MIM-ESI MS is applicable for the direct quantitation of pesticide residues in CHMs. This detection technology may help to ensure the quality of CHMs in the future.
Being abundant and active, Fe2O3 is suitable for selective oxidation of H2S. However, its practical application is limited due to the poor sulfur selectivity and rapid deactivation. Herein, we report a facile template-free hydrothermal method to fabricate porous α-Fe2O3/SnO2 composites with hierarchical nanoflower that can obviously improve the catalytic performance of Fe2O3. It was disclosed that the synergistic effect between α-Fe2O3 and SnO2 promotes the physico-chemical properties of α-Fe2O3/SnO2 composites. Specifically, the electron transfer between the Fe2+/Fe3+ and Sn2+/Sn4+ redox couples enhances the reducibility of α-Fe2O3/SnO2 composites. The number of oxygen vacancies is improved when the Fe cations incorporate into SnO2 structure, which facilitates the adsorption and activation of oxygen species. Additionally, the porous structure improves the accessibility of H2S to active sites. Among the composites, Fe1Sn1 exhibits complete H2S conversion with 100% sulfur selectivity at 220 ℃, better than those of pure α-Fe2O3 and SnO2. Moreover, Fe1Sn1 catalyst shows high stability and water resistance.
Owing to the special formation of photopolymerized hydrogels, they can effectively control the formation of hydrogels in space and time. Moreover, the photopolymerized hydrogels have mild formation conditions and biocompatibility; therefore, they can be widely used in tissue engineering. With the development and application of manufacturing technology, photopolymerized hydrogels can be widely used in cell encapsulation, scaffold materials, and other tissue engineering fields through more elaborate manufacturing methods. This review covers the types of photoinitiators, manufacturing technologies for photopolymerized hydrogels as well as the materials used, and a summary of the applications of photopolymerized hydrogels in tissue engineering.