Visible-light-induced,autopromoted nickel-catalyzed three-component arylsulfonation of 1,3-enynes and mechanistic insights

Science China Chemistry - A light-induced, nickel-catalyzed three-component arylsulfonation of 1,3-enynes in the absence of photocatalyst is reported. This methodology exhibited mild conditions,...     

Evaluation of green and efficient deep eutectic solvents as media for extracting alkaloids from lotus leaf

Deep eutectic solvents (DESs) were applied as eco-friendly solvents in this study for the extraction of alkaloids from lotus leaf, including O-nornuciferine, N-nornuciferine, nuciferine and roemerine. A series of hydrophilic and hydrophobic DESs with different hydrogen bond donors and a acceptors were synthesized and screened for a suitable DESs for extraction of alkaloids from lotus leaf. The study results showed that the hydrophilic DES with choline chloride and propanediol had the highest extraction yield. The main factors affecting the extraction efficiency—choline chloride–propanediol ratio, water content in deep eutectic solvents, solid–liquid ratio and extraction time—were investigated via a single-factor experiment. The optimized extraction conditions were 30% of water in choline chloride–propanediol (1:4) for heated extraction for 30 min and solid–liquid ratio 1:100 g/ml. Under optimum conditions, the extraction yields of O-nornuciferine, N-nornuciferine, nuciferine and roemerine were 0.069, 0.152, 0.334 and 0.041 g/100 g respectively, which were higher than those of methanol in acidified aqueous solution. This study suggests considerable potential for DESs as promising materials for the green and efficient extraction solvents for bioactive alkaloids from natural sources.     

A posteriori error analysis of a quadratic finite volume method for nonlinear elliptic problems

In this article, we construct and analyze a residual-based a posteriori error estimator for a quadratic finite volume method (FVM) for solving nonlinear elliptic partial differential equations with homogeneous Dirichlet boundary conditions. We shall prove that the a posteriori error estimator yields the global upper and local lower bounds for the norm error of the FVM. So that the a posteriori error estimator is equivalent to the true error in a certain sense. Numerical experiments are performed to illustrate the theoretical results.     

Enhanced Power Density of Alcohol Biofuel Cell by Polymer-assisted Crosslinks of 3D Graphene on Carbon Paper as the Bioanode

Herein, we successfully construct the 3D biocompatible graphene through crosslinking 2D graphene nanosheet onto carbon fiber paper with poly(diallyldimethylammonium chloride) (PDDA) as anode of the alcohol biofuel cell. Compared with the bioanode without 3D graphene, the current density and output power of PDDA-graphene-ADH bioanode is increased by 23 % and 41 % at a high concentration of ethanol at pH 8.9, suggesting the stabilization role of graphene in enzyme loading. The study provides us a deep analysis on structures and performances of the bioanode incl. electrochemistry, X-ray photoelectron spectra, and atomic force microscopy images, which is significant to develop the new methods to construct 3D porous electrodes in energy conversion device.     

Characterization of diterpene metabolism in rats with ingestion of seed products from Euphorbia lathyris L. (Semen Euphorbiae and Semen Euphorbiae Pulveratum) using UHPLC-Q-Exactive MS

Previous pharmacological studies have indicated that diterpenoids are the primary effective chemical cluster in the seeds of Euphorbia lathyris L. The seed products are used in traditional Chinese medicine in the forms of Semen Euphorbiae (SE) and Semen Euphorbiae Pulveratum (SEP). However, the metabolism of the plant's diterpenoids has not been well elucidated, which means that the in vivo metabolite products have not been identified. The current study screened the physiological metabolites of six diterpenes [Euphorbia factor L₁ (L1), L₂ (L2), L₃ (L3), L_7a (L7a), L_7b (L7b), and L₈ (L8)] in feces and urine of rats after oral administration of SE and SEP using UHPLC-Q-Exactive MS. A total of 22 metabolites were detected in feces and 8 in urine, indicating that the major elimination route of diterpenoids is via the colon. Hydrolysis, methylation, and glucuronidation served as the primary metabolic pathways of these diterpenoids. In sum, this study contributed to the elucidation of new metabolites and metabolic pathways of SE and SEP, and the new chemical identities can be used to guide further pharmacokinetic studies.     

One-pot,one-step,and selective terpolymerization of ethylene oxide,propylene oxide,and COS to copoly(thioether)s with tunable thermal properties

Facile construction of sulfur-rich polymers using readily available raw chemicals is an area aggressively pursued but challenging. Herein we use common feedstocks of ethylene oxide (EO), propylene oxide (PO), and carbonyl sulfide (COS) to synthesize copoly(thioether)s which are traditionally produced from unpleasant and difficult to store episulfides. In this protocol, the EO/COS coupling selectively generates a pure poly(ethylene sulfide) (PES) with melting temperature (T_m) values up to 172°C and high yields up to 98%. The EO/PO/COS terpolymerization leads to the incorporation of soft poly(propylene sulfide) (PPS) and hard PES segments together, affording a random PES-co-PPS copoly(thioether) with the complete consumption of EO and PO. Additionally, by simply varying the EO/PO feeding ratio, the obtained copoly(thioether)s possess tunable thermal properties, T_m values in the range of 76–144°C, and excellent solubility. These copolymerizations are conducted in one-pot/one-step at industrially favored reaction temperatures of 100–120°C using catalysts of common organic bases, suggesting a facile and practical manner. Especially, the copoly(thioether) exhibits high refractive indices up to 1.68 owing to its high sulfur content, suggesting a broad application prospect in optical materials.     

Solar light-driven photocatalytic production of hypochlorous acid over Pt/WO3 in seawater for marine antifouling

The hypochlorous acid (HCIO) was synthesized from seawater by the Pt/WO₃ photocatalyst under visible-light irradiation. The effect of WO₃ morphology and Pt loading on the performance of the composite photocatalyst for the production of HCIO has been studied in detail. The study found that among the series of materials, hollow WO₃ microspheres with a diameter of about 3 μm loaded with 1.0 wt% Pt have the best HCIO production performance. Over it, 14.52 μM of HClO (1.24 mg/L of free chlorine) was accumulated in 0.5 M NaCl solution after 2 h of visible-light photoirradiation. What is more, the concentration of HClO can reach 4.34 μM (0.354 mg/L free chlorine) in natural seawater for 1 h using this Pt/WO₃ photocatalyst. Under visible-light irradiation, the Pt/WO₃ photocatalyst has a good broad-spectrum antibacterial activity and the activity of inhibiting marine fouling algae. The Pt/WO₃ photocatalyst has high stability and reusability. All these characteristics are conducive to the application in the field of marine antifouling. Moreover, the photocatalytic reaction mechanism was evaluated by studying the photoelectrochemical properties of Pt/WO₃/FTO. This research provides a new strategy for replacing the traditional electrolytic marine antifouling system with the visible-light-catalyzed HClO production system.

     

Injectable and self-healing hydrogels with tissue adhesiveness and antibacterial activity as wound dressings for infected wound healing

The design of wound dressings with excellent self-healing ability, adequate adhesion, good biocompatibility, and potential antibacterial ability is of great significance for the healing of infected wounds arising from human activities. Herein, a series of multi-functional hydrogel dressings, poly(ionized isocyanoethyl methacrylate-glutamine)/poly(hexamethylene guanidine) (iG_x/PHMG_y) hydrogels, were obtained through homopolymerization of fully ionized isocyanoethyl methacrylate-glutamine (iIEM-Gln) in the presence of poly(hexamethylene guanidine) (PHMG), in which strong hydrogen bonds were formed among urea groups in the P (iIEM-Gln) chain to form a stable hydrogel network. The prepared iG_x/PHMG_y hydrogels exhibited adequate self-healing ability and tissue adhesion, which could be firmly adhered to the wound surface and remained intact during application. In addition, the presence of PHMG imparted good antibacterial activity to the hydrogels for the effective promotion of the wound healing in S. aureus infected skin wound on mice. Overall, this multi-functional hydrogel provides a facile and effective strategy for the design of infected wound dressings, and may show great potential in clinical applications.     

Surface Engineering of Conjugated Polybenzothiadiazoles and Integration with Cobalt Oxides for Photocatalytic Water Oxidation

Conjugated polymers feature promising structure and properties for photocatalytic water splitting. Herein, a hydrolysis strategy was demonstrated to rationally modulate the surface hydrophilicity and band structures of conjugated poly-benzothiadiazoles. High hydrophilicity not only enhances the dispersions of polymeric solids in an aqueous solution but also reduces the absorption energy of water molecules. Besides, both theoretical and experimental results reveal that a more positive valence band potential is generated, which contributes to enhancing the photocatalytic water oxidation performance. Accordingly, the surface-modified conjugated polymers show largely promoted photocatalytic water oxidation activities by deposition of cobalt oxides as cocatalysts.     

Guaranteed cost positive consensus for multi-agent systems with multiple time-varying delays and MDADT switching

Nonlinear Dynamics - This paper investigates the guaranteed cost positive consensus for linear multi-agent systems (MASs) with multiple time-varying delays and switching topologies. First,...