A series of cyclohexanones substituted at the 4-position with a selection of hydrophobic and hydrophilic groups were used as substrates in the evaluation of six new cyclopentanone monooxygenase (CPMO) mutants. These mutants were obtained through evolutionary modifications in two specific regions of the CPMO’s putative active site. Several mutant enzymes with improved enantioselectivity were identified. Analysis of the results, in terms of a diamond model, illustrates how a family of cyclohexanone substrates may be used to explore putative active sites of Baeyer–Villiger monooxygenases (BVMOs) and to design productive mutations for specific substrates. 相似文献
A Sc(OTf)3-catalyzed [3 + 3] cycloaddition of 2,2′-diester aziridines with β-(indol-2-yl)-α,β-unsaturated ketones was developed, affording polysubstituted tetrahydro-γ-carbolines in single diastereoisomers in good to excellent yields. 相似文献
The excessive production and deposition of amyloid-β (Aβ) is one of the most important etiologies of Alzheimer''s disease (AD). The interaction between Aβ and metal ions produces aberrant reactive oxygen species (ROS), which induce oxidative stress and accelerate the progression of AD. To reduce Aβ plaques and ROS to maintain their homeostasis is an emerging and ingenious strategy for effective treatment of AD. Herein, we report the rational design of multifunctional micelles (MPGLT) based on a polymer-grafted peptide to simultaneously clear Aβ and ROS for AD therapy. The MPGLT integrating three functional peptides as a ROS scavenger (tk-GSH), β-sheet breaker (LP) and an autophagy activator (TK) respectively, could capture and degrade Aβ. Meanwhile, the tk-GSH on the surface of MPGLT effectively scavenges the intracellular ROS. Consequently, MPGLT reduced the cytotoxicity of Aβ and ROS. In vivo animal studies using an AD mouse model further showed that MPGLT could transport across the blood–brain barrier for decreasing the Aβ plaque and eliminating ROS in vivo. This peptide micelle-based synergistic strategy may provide novel insight for AD therapy.Multifunctional micelles based on a peptide–polymer for simultaneously targeting Aβ degradation and ROS scavenging for AD therapy. 相似文献
Carbon quantum dots (CQDs) co-doped with N, P and S derived from expired milk was prepared by a simple hydrothermal method. By dipping pure cotton face towel (PCFT) into CQDs ink, a flexible all-biomass CQDs/PCFT sensor was prepared for the first time. Due to the heteroatom doping, extremely small particle size of CQDs and excellent permeability of CQDs/PCFT film, the flexible CQDs/PCFT sensor showed the high sensitivity and bending stability. In the range of 0–60° bending states, the responses of CQDs/PCFT sensor to four target analytes changed by less 5.0%. After 3000 bending of 60°, the maximum change of the response to the target analytes was only 6.4%. Interestingly, due to the abundant functional groups and defects of CQDs, the flexible CQDs/PCFT sensor displayed sensing curves of different shapes for different target analytes. In this way, by establishing a database of sensing curves of target analytes, multiple analytes can be detected discriminatively by relying only on single sensor with the help of image recognition. This work provided a reference for the development of cotton fiber based all biomass flexible gas sensor.
Ti_3C_2 belongs to MXenes family,which is a new two-dimensional material and has been applied in many fields.With simple method of hydrothermal and high temperature calcination,nano structured Ni/Ti_3C_2T_x hybrid was synthesized.The stable layer structure of Ti_3C_2 MXene providing high surface area as well as excellent electronic conductivity are beneficial for deposition and decomposition of discharge product Li_2O_2.Furthermore,possessing special catalytic activity,Ni nanoparticles with size of about 20 nm could accelerate Li_2O_2 breaking down.Taking advantage of two kinds of materials,Ni/Ti_3C_2T_x hybrid as cathode of Li-O_2 battery can achieve a maximal specific capacity of 20,264 mAh/g in 100 mA/g and 10,699 mAh/g in 500 mA/g at the first cycle.This work confirms that the prepared Ni/Ti_3C_2T_x hybrid exhibiting better cycling stability points out a new guideline to improve the electrochemical performance of lithium-oxygen batteries. 相似文献
The macromolecular structure of humic substances (HS), i.e. molecular size, shape, conformation, and weight is believed to control key physico-chemical reactions in aquatic systems. However, these properties of HS are still deeply a matter of debate. Furthermore, they are affected by solution physico-chemical parameters such as ionic strength, pH, and chemical composition, etc. To better understand aggregation processes of HS in natural waters, the effects of cation concentration and type, water composition, and pH on the size and conformation of the Suwannee River Humic Acid (SRHA) were investigated with synthetic solutions. The size and the conformation of the SRHA in NaCl and CaCl2 solutions at different concentrations (0.001–0.5 M) and pH (4.5–9.3) were determined using the photon correlation spectroscopy (PCS) and transmission electron microscopy (TEM), respectively. In addition, dissolved organic matter (DOM) samples collected from the Adour estuary along a salinity gradient were imaged by TEM. The average size of the SRHA measured by PCS increased with pH and ionic strength. This behavior was confirmed by TEM micrographs. The increase in pH and CaCl2 engendered aggregation of the SRHA. Two aggregation steps were identified, a big increase in HS size occurred for small changes in CaCl2 concentrations in the range <0.02 M CaCl2, and a slight increase occured for higher concentrations in the range >0.02 M CaCl2. The parallel analysis of SRHA by PCS and TEM allowed overcoming the limits for both techniques.Comparable results were found for the DOM samples from the Adour estuary (South West of France). The conformation and size of the HS network of these samples varied with the salinity gradient. TEM images demonstrated that, HS have a branched open network in freshwater whereas they have a more compacted and close network with increasing salinity. 相似文献
Two novel complexes {[Co(A-glu)(Im)2]·0.5H2O}n (1) and [Cd(A-glu)(Im)3]n (2) (H2A-glu=N-acetyl-L-glutamic acid, Im=imidazole) have been synthesized from the reaction of H2A-glu with Co(CH3COO)2·4H2O or Cd(CH3COO)2·2H2O in the presence of Im. Both of the complexes display different coordination environment and similar one-dimensional chain structure. The magnetic susceptibility measurements for 1 show a weak antiferromagnetic interaction between two cobalt(Ⅱ) ions bridged by A-glu ligand. The complex 2 exhibits an intense fluorescent emission in solid state at room temperature. 相似文献
An acid-mediated multicomponent reaction has been developed for the direct synthesis of multifused 1,3-benzoxazine derivatives from simple and readily available arylglyoxal monohydrates and 2-aminobenzyl alcohols under mild conditions. This novel protocol is proposed to proceed through intramolecular poly-heterocyclizations, thus leading to the formation of three new rings and six new chemical bonds, including four CN and two CO bonds. 相似文献