Latest ArticlesHighly enantioselective Rh-catalyzed partial hydrogenation of unprotected simple 2-alkyl-5-aryl-disubstituted pyrroles has been successfully developed, generating a series of chiral 1-pyrroline derivatives generally with excellent results (95%–99% yields, 91%–96% ee). Moreover, 2,5-aryl-1H-pyrroles were hydrogenated well in high yields and good enantioselectivities. This efficient protocol features easily accessible substrates, wide substrate scope, well functional group compatibility, commercially available rhodium precursor and chiral ligand. It provides a versatile route to access chiral 1-pyrroline derivatives that are of great importance in organic synthesis and pharmaceutical chemistry.
Nanoscale low-dimensional chiral architectures are increasingly receiving scientific interest, because of their potential applications in many fields such as chiral recognition, separation and transformation. Using 6, 12-dibromochrysene (DBCh), we successfully constructed and characterized the large-area two-dimensional chiral networks on Au(111) and one-dimensional metal-liganded chiral chains on Cu(111) respectively. The reasons and processes of chiral transformation of chiral networks on Au(111) were analyzed. We used scanning tunneling spectroscopy (STS) to analyze the electronic state information of this chiral structure. This work combines scanning tunneling microscopy (STM) with non-contact atomic force microscopy (nc-AFM) techniques to achieve ultra-high-resolution characterization of chiral structures on low-dimensional surfaces, which may be applied to the bond analysis of functional nanofilms. Density functional theory (DFT) was used to simulate the adsorption behavior of the molecular and energy analysis in order to verify the experimental results.
Target discovery, involving target identification and validation, is the prerequisite for drug discovery and screening. Novel methodologies and technologies for the precise discovery and confirmation of drug targets are powerful tools in understanding the disease, looking for a drug and elucidating the mechanism of drug treatment. Among the common target identification and confirmation methods, the modified method is time-consuming and laborious, which may reduce or change the activity of natural products. The unmodified methods developed in recent years without chemical modification have gradually become an important means of studying drug targets. A wide range of unmodified approaches have been reported, introducing and analyzing the recent emerging methodologies and technologies. This review highlights the advantages and limitations of these methods for the application of drug target discovery and presents an overview of their contributions to the target discovery of small molecule drugs. The application and future development trends of methodologies in target discovery are also prospected to provide a reference for drug target research.
Hydrogen peroxide (H2O2) synthesis generally involves the energy-intensive anthraquinone process. Alternatively, electrochemical synthesis provides a green, economical, and environmentally friendly route to prepare H2O2 via the two-electron oxygen reduction reaction, but this process requires efficient catalysts with high activity and selectivity simultaneously. Here, we report an N, O co-doped carbon xerogel-based electrocatalyst (NO-CX) prepared by a simple and economical method. The NO-CX catalyst exhibits a high H2O2 selectivity over 90% in a potential range of 0.2–0.6 V and a high H2O2 production rate of 1410 mmol gcat−1 h−1. The density functional theory calculations demonstrate that the coupling effect between N and O can effectively induce the redistribution of surface charge and the edge carbon atom adjacent to an ether group and a graphite nitrogen atom is the active site. This work provides a straightforward and low-cost process to produce highly selective H2O2 catalysts, which is in place for the expansion of electrocatalytic synthesis of useful chemicals.
Two-dimensional polymers (2DPs) are emerging crystalline 2D organic material comprising free-standing, single-atom/monomer-thick, planar, and covalent networks with long-ranging structural order. Benefiting from their intrinsic porosity, crystallinity, and electrical properties, 2DPs have displayed great potential for separation, energy conversion and electronic fields. In this mini review, we aim to provide the recent progress in crystalline 2DPs films form synthesis strategies to characterization methods, as well as the future trends. We first present the synthesis strategy of single-crystalline 2DPs films including crystal engineering approaches and surface science. Also, we summarize the characterization methods of 2DPs films and highlight the advantages and limitations of different methods focusing on chemical bonding, morphology, and crystal structure. Finally, we will present the current challenges and trends regarding the future developments of crystallinity, monomer design, synthesis strategy and characterization.
Understanding and establishing the structure-activity relation of nanoparticles is a prerequisite for rational design of high-performance electrocatalysts. Cu2O nanoparticles enclosed with different crystal facets, namely, o-Cu2O NPs with {111} facets, c-Cu2O NPs with {100} facets are prepared and their electrocatalytic properties for oxygen evolution reaction (OER) in alkaline condition are evaluated at single nanoparticle level with a combination of scanning electrochemical cell microscopy and scanning electron microscopy. It is found that the o-Cu2O NPs have significantly superior OER electrocatalytic activity compared to c-Cu2O, which is almost inert. The estimated turnover frequency (TOF) at 1.97 V vs. RHE on {111} facet increases from 4 s−1 to 115 s−1 with the octahedron edge length decreasing from 1.3 µm to 100 nm. Deposition of carbon on c-Cu2O surface barely promotes the activity, suggesting the inherent poor electric conductivity within the nanocrystal is most likely the reason for low activity. This work provides direct probing to single transition metal oxide crystals with dramatically different activity.
Metal-organic frameworks (MOFs) materials with highly ordered and porous crystalline structure, have excellent performance in advanced oxidation progresses (AOPs) for organic contaminants degradation in water treatment. This review intends to summarize the timely references and insights for the recent advances in MOFs that are used in AOPs. Starting with the preparation methodologies, including conventional hydrothermal method, electrochemical method, sol-gel method, and emerging microwave and ultrasound assisted synthesis methods. Application and mechanism for MOFs using in various AOPs of Fenton-like, photocatalysis, catalytic ozonation, persulfate catalysis and other emerging oxidation methods are emphatically discussed. We hope this review can comprehensively summarize the research and application progress of MOFs in AOPs, deepen the understanding of the catalytic mechanisms.
A stimuli-responsive supramolecular polymer network has been constructed based on the host-guest interactions between the copolymer poly-P[5]A with pendent pillararene units and bis(sulfonium) diction guest G2. The formation mechanism of the supramolecular polymer network has been explored by the intensive study. With the addition of the competitive molecules and heating, the supramolecular polymer network could be dissociated and lead to clear changes in NMR spectroscopy and viscosity property.
Diabetic wounds lead to a decrease in quality of life and an increase in mortality. Current treatment strategies include preventing bacterial adhesion while improving microcirculation. As a new type of wound dressing that imitates natural skin, hydrogel has gradually emerged with its excellent properties. However, existing hydrogels rarely achieve satisfactory results in promoting wound repair and antibacterial simultaneously. In this case, we prepared methacrylic anhydride chemically modified hyaluronic acid as a hydrogel matrix, added polyhexamethylene biguanide as an antibacterial component, and loaded sodium alginate/salidroside composite microspheres which could sustainably release salidroside and thus promote angiogenesis. Hybrid hydrogel (HAMA/PHMB-Ms) was synthesized via photocrosslinking, and its chemical structure, particle size distribution and microstructure were characterized. The satisfactory antibacterial properties of the HAMA/PHMB(15%)-Ms hydrogel were studied in vitro, and its antibacterial rates against E. coli and S. aureus were 97.85% and 98.56%, respectively. In addition, after demonstrating its good biocompatibility, we verified that the HAMA/PHMB-Ms hydrogel has increased granulation tissue formation, more collagen deposition, more subcutaneous capillary formation, and better wound healing than blank control, HAMA and HAMA/PHMB hydrogel on the back wound model of diabetic mice. The results confirmed that HAMA/PHMB-Ms hydrogel was a promising material for the treatment of the diabetic wounds.
Cascading reactions in fluorophores accompanied by the replacement of different fluorescence wavelengths can be used to develop luminescent materials and reactive fluorescent probes. Based on multiple signal channels, the selectivity of probes can be improved and the range of response to guest molecule recognition can be expanded. By regulating the position, number, and activity of active sites in fluorophores, fluorescent probes that successively react with thiol and amino groups in cysteine (Cys), homocysteine (Hcy) have been developed, which can only react with the thiol group of GSH. In this paper, we report the first probe capable of cascading nucleophilic substitution reaction with the thiol group and amino group of GSH at a single reaction site, and showed the dual-color recognition of GSH, which improved the selectivity of GSH also was an extension of GSH probes. The probe Rho-DEA was based on a TICS fluorophore, and the intramolecular cascade nucleophilic substitution reaction occurs with Cys/Hcy. The thiol substitution of the first step reaction with Cys/Hcy was quenched due to intersystem crossing to triplet state, so GSH can be selectively recognized from the fluorescence signal. Rho-DEA has the ability of mitochondrial localization, and finally realized in situ dual-color fluorescence recognition of GSH in mitochondria.
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