Latest ArticlesCytochrome P450 OleTSA, a new cytochrome P450 enzyme from Staphylococcus aureus, catalyzes the oxidative decarboxylation and hydroxylation of fatty acids to generate terminal alkenes and fatty alcohols. The mechanism of this bifurcative chemistry remains largely unknown. Herein, a class of derivatized fatty acids were synthesized as probes to investigate the effects of substrate structure on the product type of P450 OleTSA. The results demonstrate that the fine-tuned structure of substrates, even in a remote distance from the carboxyl group, significantly regulates OleT catalyzed decarboxylation/hydroxylation reactions. Molecular docking analysis indicated the potential interactions between the carboxylate groups of different probes and the enzyme active center which was attributed to the bifurcative chemistry.
Acephate pesticide contamination in agricultural production has caused serious human health problems. Metal oxide semiconductor (MOS) gas sensor can be used as a portable and promising alternative tool for efficiently detection of acephate. In this study, hierarchical assembled SnO2 nanosphere, SnO2 hollow nanosphere and SnO2 nanoflower were synthesized respectively as high efficiency sensing materials to build rapid and selective acephate pesticide residues sensors. The morphologies of different SnO2 3D nanostructures were characterized by various material characterization technology. The sensitive performance test results of the 3D SnO2 nanomaterials towards acephate show that hollow nanosphere SnO2 based sensor displayed preferable sensitivity, selectivity, and rapid response (9 s) properties toward acephate at the optimal working temperature (300 ℃). This SnO2 hollow nanosphere based gas sensor represents a useful tool for simple and highly effective monitoring of acephate pesticide residues in food and environment. According to the characterization results, particularly Brunauer-Emmett-Teller (BET) and Ultraviolet-Visible Spectroscopy (UV–vis), the obvious and fast response can be attributed to the mesoporous hollow nanosphere structure and appropriate band gap of SnO2 hollow nanosphere.
Heavy oil is treated as an undesirable raw material in traditional refining markets because of its low yield. However, its rich natural aromatic structure and heteroatomic compounds make it possible to be a precursor to large-scale production of carbon materials. Using heavy oil and three SDA products as precursors, we synthesized highly fluorescent multi-color carbon dots (CDs) by hydrothermal method, which can precisely control the photoluminescence wavelength in the range of 350−650 nm. The synthesized carbon dots have the advantages of good long-term stability and stability under extreme pH conditions and low price. Importantly, the carbon dots synthesized with asphalt as the precursor have the highest fluorescence quantum yield. X-ray photoelectron spectroscopy (XPS) is used to elucidate the effects of different precursor on emission color change and photoluminescence quantum yield (PLQY), thus providing a controlled tuning of the system for the functionalization of CDs. And we further used the CDs in macrophage labeling. This pathway gives a reliable and repeatable industry possibility and may boost the applications of CDs into reality.
A Ru(Ⅱ)-catalyzed para-difluoroalkylation of aromatic aldehydes and ketones with a transient directing group has been developed. It utilizes less expensive ruthenium catalysts and allows facile access to challenging difluoroalkylated aldehydes. The mechanism studies suggest that the distinct coordination mode of ruthenium complex with imine moieties is responsible for para-selectivity.
Studies on the synthesis of antifungal and anticancer natural product, pseudolaric acid B, have led to the enantioselective synthesis of di-epi-trans-fused [5–7]-bicyclic core skeleton. The synthesis was achieved in 10 linear steps, which features the Sharpless asymmetric epoxidation, cyanide-opening reaction of epoxide, and intramolecular [5+2] cycloaddition reaction as the key transformations. The stereochemistry was determined by the X-ray crystallographic analysis.
The asymmetric transfer hydrogenation (ATH) of a wide range of ketones catalyzed by manganese complex as well as chiral PxNy-type ligand under mild conditions was investigated. Using 2-propanol as hydrogen source, various ketones could be enantioselectively hydrogenated by combining cheap, readily available [MnBr(CO)5] with chiral, 22-membered macrocyclic ligand (R, R, R', R')-CyP2N4 (L5) with 2 mol% of catalyst loading, affording highly valuable chiral alcohols with up to 95% ee.
Helix structures at atomic/molecular level have not been found in self-assembled peptide sequence with less than three residues. As β-sheet supramolecular secondary structures have been discovered in solid-state amino acids, we here report the conjugation of simple N-terminal aryl protecting group could give rise to helical supramolecular secondary structures in solid-state, which determines the optical activities of the adjacent aryl groups. The carboxylic acid-involved asymmetric H-bonds in N-terminal aryl amino acids induce the emergence of super-helical structures of amino acid residues and aryl groups. In most cases, supramolecular tilted chirality of aryl groups is opposite to that of amino acid sequences, of which handedness and helical pitch are determined by the H-bond modalities. Determining correlation between supramolecular tilted chirality of aryl segments and their chiroptical activities is firstly unveiled, which was verified by the computational results based on density functional theory. Most aryl amino acids self-assembled by nanoprecipitation method via crystallization induced self-assembly into rigid one-dimensional microstructures with ultra-high Young's modulus. This study reveals the generic existence of chiral supramolecular structures in aggregated amino acid derivatives and gives an in-depth investigation into the structural-property relationships, which could guide the rational design and screening of chiroptical supramolecular materials.
Phosphatase plays a vital important role in many biological functions due to the dephosphorylation serves varied roles in cellular regulation and signaling. Among the family of phosphatase, alkaline phosphatase (ALP) could act as crucial prognostic indicators for many diseases such as bone diseases and cancer. However, the detection of ALP is mainly limited to in vitro colorimetric method in clinic. Therefore, huge efforts have been paid on the fluorescence imaging that provides a reliable method to detect the real-time and in vivo changes of the level of ALP. In this review, we summarize recent advances in fluorescence imaging of phosphatase, mainly focused on ALP. The imaging probes of phosphatase are mainly classified according to their luminescence mechanisms. In the end, we assessed the challenges and future prospects of phosphatase probes.
The utilization of thermal energy from different sources is an important development direction for conserving energy. With the development of technology, refined and rapid utilization of thermal energy is required. Traditional thermal conductive materials cannot meet the growing needs of human beings. Therefore, people pay attention to two-dimensional graphene film materials for their thermal conductivity. This review collects current modeling group of thermal transport on graphene, including non-equilibrium Green function (NEGF) theory, molecular dynamics (MD) simulations modeling and Boltzmann transport equation method. These models can well explain several phenomena of phonon transport in graphene. Further, structural defects were discussed and expounded the effect for graphene thermal conductivity, including doping, grain boundary and defects. Deeply understanding of defects on graphene, we can better grasp the thermal conductivity of graphene from the microscopic point of view.
Delivery systems based on nanoparticles (NPs) have shown great potential to reduce side effects and improve the therapeutic efficacy. Herein, we report the one-pot synthesis of poly(ethylene glycol)-mediated zeolitic imidazolate framework-8 (ZIF-8) NPs for the co-delivery of an anticancer drug (i.e., doxorubicin) and a cell penetrating peptide containing histidine and arginine (i.e., H4R4) to improve the efficacy of therapeutic delivery. The cargo-encapsulated ZIF-8 NPs are pH-responsive, which are stable at neutral pH and degradable at acidic pH to release the encapsulated cargos. The released H4R4 can help for endosome/lysosome escape to enhance the cytotoxicity of the encapsulated drugs. In vivo studies demonstrate that the co-delivery of doxorubicin and H4R4 peptides can efficiently inhibit tumor growth without significant side effects. The reported strategy provides a new perspective on the design of drug delivery systems and brings more opportunities for biomedical applications.
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