Latest ArticlesTreatment of antibiotics contaminated water remains a global environmental challenge. In this study, tetracycline (TC) was found to effectively sensitize pure TiO2 for visible light photocatalytic degradation via a ligand-to-metal charge transfer mechanism. The sensitization was attributed to the formation of TC-TiO2 complex and the overlap of the molecular orbitals of TC and the conduction band of TiO2. The intermediate degradation products of TC, however, did not sensitize TiO2, which was the reason for the low mineralization rate. Nevertheless, our results showed that the intermediate degradation products of TC had significantly reduced bactericidal effects and less induction of antibiotic-resistance genes (ARGs). This study showcases an effective treatment of antibiotics-containing wastewater using the most common photocatalyst TiO2 with reduced risk in the spread of ARGs.
Advanced oxidation processes (AOPs) are promising technology to remove organic pollutant in water. However, the main problem in the AOPs is the low generation of hydroxyl radical (•OH) owing to the low decomposition efficiency of hydrogen peroxide (H2O2). Herein, the spinel type cobalt acid manganese (MnCo2O4) with flower morphology was fabricated through a co-precipitation method. In situ Fourier transform infrared spectroscopy confirms that the MnCo2O4 with the optimal molar ratio of Co and Mn precursors (CM3, Co: Mn = 3) has more Lewis acid sites compared with single metal oxide catalysts (Co3O4 and Mn2O3), leading to the excellent performances for H2O2 decomposition rate constant on CM3, which is about 15.03 and 4.21 times higher than those of Co3O4 and Mn2O3, respectively. As a result, the obtained CM3 shows a higher ciprofloxacin degradation ratio than that of Co3O4 and Mn2O3. Furthermore, CM3 shows an excellent stability during several cycles. This work proposes effective catalysts for ciprofloxacin decomposition and provides feasible route for treating practical environmental problems.
A calix[4]arene ligand assisted direct β-C−H arylation of tertiary aliphatic aldehydes has been developed via a Pd-catalyzed C(sp3)−H functionalization process. This strategy exhibited good functional group compatibility and C−H bond site-selectivity. Mechanism studies have shown that both synergistic effect and cationic-π supramolecular interaction between calixarene cavity and transition-metal catalytic center may play an important role in this catalytic cycle. This complementary method would be used in organic and medical chemistry due to the importance of tertiary aliphatic aldehydes.
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 novel Mo-doped CuO catalyst is developed and used for low-temperature NH3-SCR reaction. Compared with the undoped CuO sample, the Mo doped CuO catalyst shows an increased SCR performance with above 80% NOx conversion at 175 ℃. The XRD and Raman results have confirmed the incorporation of Mo metal ions into CuO lattice to form Mo-O-Cu species which may be related to the enhanced SCR activity. The XPS and UV–vis results reveal the creation of electron interaction between Cu and Mo in this Mo-O-Cu system which provides an increased amount of Lewis and Brønsted acid sites, thereby promoting the adsorption capacity of NH3 and NOx as verified by NH3-TPD and NOx-TPD characterization. Besides, it also promotes the formation of oxygen vacancies, leading to the increasing of chemisorbed oxygen species, which improves the NO oxidation to NO2 activity. Furthermore, in situ DRIFTS technology was also used to study the reaction mechanism of this Mo doped CuO catalyst. The formed NO2 could react with NHx (x = 3, 2) species to enhance the low-temperature NH3-SCR activity via the "fast-SCR" reaction pathway. The nitrate and nitrite ad-species may react with NH3 and NH4+ ad-species through the L-H pathway.
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.
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 sulfonated diterpenoid alkaloids possessing different but related novel carbon skeletons, named aconidenusulfonine A (1) and 12, 16-secoaconidenusulfonine A (2), respectively, were isolated as minor components from an aqueous extract of the lateral roots of Aconitum carmichaelii ("Fu Zi"). The structures of 1 and 2, representing the first two C21-diterpenoid alkaloids from nature, were determined by analysis of various spectroscopic data and chemical transformation, of which 1 was further proved by single-crystal X-ray diffraction. Especially, 1 exhibited dose-depended analgesic activity consistent with the clinical function of Fu Zi.