Latest ArticlesTwo distinctive rearranged 19-nor-7,8-seco-labdane diterpenoids (1 and 2) with a novel tetracyclo[5.2.1.02,5.04,10]decane skeleton, a derivative of the open tetrahydrofuran ring (7), three dimeric compounds (8−10), and four revised homologs (3−6) were obtained from Chinese liverwort Pallavicinia ambigua. Their structures were identified via combined analysis of their spectroscopic data, single-crystal X-ray diffraction patterns, and ECD calculations. The light-driven conversion of compound 5 to compounds 1−4 demonstrated that photochemically induced postmodification involved in biosynthesis is an important way to diversify natural structures. A preliminary cytotoxicity assay revealed that compound 5 showed significant inhibition in the human prostate cancer (PC-3) cell line via an apoptotic pathway.
The development of lithium-metal batteries (LMBs) is seriously restricted by the out-of-control dendrites growth and infinite volume expansion. Herein, a pervasive organic-inorganic layer construction strategy is reported for the composite lithium metal anode with congener-derived organic-inorganic solid electrolyte interphase (SEI). In this strategy, the organic-inorganic Ag@polydopamine (Ag@PDA) layer is coated on the arbitrary substrates by a simple two-step method. The thin and stable congener-derived SEI is in-situ formed with fewer inorganic components and more organic components during charging/discharging. The polydopamine with sufficient adhesion groups and lithiophilic Ag layer realize near-zero nucleation overpotential during lithium deposition. The low interface resistance and stable lithium deposition are achieved. Moreover, the practical areal and volumetric capacities of the composite anode with three-dimensional copper (3DCu) as the substrate are 10 mAh/cm2 and 1538 mAh/cm3 (vs. the mass of anode). The symmetrical cell shows very low polarization voltage (10 mV) and more than 2500 h cycles life at 1 mA/cm2 (1 mAh/cm2). The LiNi0.8Co0.1Mn0.1O2 (NCM811)-based full cells show improved capacity retention (82%) after 100 cycles at 0.5 C. The modified lithiophilic anode with congener-derived interphase provides a promising strategy to realize the next-generation dendrite-free LMBs.
As a common active substructure, hydrazone has attracted increasing attention and is considered essential for pesticide discovery. It has been widely regarded as a potential insecticidal, antibacterial, antifungal, antiviral, and herbicidal agent. In this review, we highlight the pesticide versatility of hydrazone fragments and provide a comprehensive summary of the biological activity, structure-activity relationship analysis (SARs), and primary mechanism of their analogs. This profile is expected to give valuable information for discovering new pesticides.
The controllable morphology and composition of catalysts are crucial to improving the electrocatalytic activity of oxygen evolution reaction (OER). Herein, we construct a bimetallic heterostructure by sulfidation and hydrothermal methods, and the layered ReS2 is vertically aligned on Prussian blue-derived hollow Co9S8 nanocubes (Co9S8@ReS2). The core-shell structure of Co9S8@ReS2 can effectively prevent the restacking of layered ReS2, expose the abundant surface area and improve the utilization of electrocatalytic sites, resulting in fast electrolyte diffusion and charge transfer during OER. Due to the synergistic effect of the core-shell morphology and the formed bimetallic heterostructure, Co9S8@ReS2 exhibits excellent catalytic OER performance. At 10 mA/cm2, only 288 mV of overpotential is required with the Tafel slope of 73.3 mV/dec for Co9S8@ReS2, which are both lower than that of Co9S8 and ReS2. Meanwhile, Co9S8@ReS2 exhibits high catalytic stability and low charge transfer resistance and the boosted active sites are confirmed by density functional theory. This work provides a rational design of the OER catalysts by constructing the bimetallic heterostructure.
Developing new functional explosives that display high stability, good energy performance, and low sensitivity are one of the key directions of energetic materials research. In this work, two-dimensional (2D) Schiff-based energetic covalent organic frameworks (COFs) are prepared based on triaminoguanidine salts with different anions as building blocks. Benefiting from the robust covalent bond in 2D extended polygons and strong π-π interactions in the eclipsed interlayers, the synthesized energetic COFs showed higher thermal stability and lower mechanical sensitivity than their precursor salts. More importantly, incorporating triaminoguanidine salts into COFs effectively increase the corrosion resistance to metal under high humidity conditions, which is due to the imine moieties in COFs functioning as π acceptors and offering strong bonding with metallic ions. This work provides a new pathway for the development of high-performance energetic materials.
Owing to the anaerobic metabolism in the tumor, abundant acidic metabolites are produced and accumulated in the cells. Therefore, the cells in different tumor layers are directly linked to the pH micro-environment. Nevertheless, due to the lack of robust tools, the high-efficient evaluation of the acidic micro-environment of tumor stratification faces the challenge of accurate diagnosis. We designed a new pH sensitive fluorescent lifetime probe target to lysosomes. As we expected, the fluorescence lifetime of PLN possesses a good linear fit to the pH value, which could detect the pH change at a single lysosome level in real time, and then evaluate the different acidity of tumor stratification. The probe PLN is successfully used to evaluate the tumor stratification by fluorescence lifetime imaging microscopy (FLIM) for the first time, which is of great significance in the preoperative diagnosis of clinical tumor treatment or evaluation of drug delivery effect.
Catalytic Michael addition reaction represents a fundamental importance in organic synthetic chemistry. Whereas corresponding conversions toward intrinsically low reactive enamide remains an ongoing challenging. We herein report a copper-catalyzed conjugate addition of allenes to β-substituted alkenyl amides, one of the most challenging Michael acceptors. The present method utilizes readily available allenes as the latent carbon-based nucleophiles and simple, common β-substituted alkenyl amides as starting materials, unlike previous methods that usually preinstall an activating group to improve the reactivity of amide or uses highly reactive stoichiometric quantities of organometallics. Hence, this approach shows good functional group compatibility and can be implemented under mild reaction conditions with excellent level of chemo- and regioselectivities.
Adenine is an essential building block of genetic material and a range of coenzymes. Chemical probes containing an adenine moiety have been used in kinase profiling studies in cell lysates. Here we report that adenine-derived small-molecule probes with an activated ester reactive group can covalently modify a conserved lysine residue of protein kinases and capture a number of nucleotide-binding proteins within living cells.
Combining phototherapy and chemotherapy has been considered a promising modality for cancer therapy due to their synergistic effect. Herein, we developed three D-π-A-structured boron dipyrromethenes (BODIPYs) (named as B-B, B-C, and B-C-Pt). Due to their enlarged π-conjugated structure and high intramolecular charge transfer effect, the synthesized BODIPYs had photothermal conversion capability, and their absorption and fluorescence spectra were red-shifted. The cisplatin-appended BODIPY (B-C-Pt) exhibited good singlet oxygen (1O2) generation ability and near infrared (NIR) absorption and fluorescence (λAbs = 748 nm, λEm = 947 nm). After being encapsulated by distearoyl phosphoethanolamine polyethyleneglycol 2000 (DSPE-PEG-2000), which could inhibit the H-aggregation of B-C-Pt, the absorption and fluorescence of the obtained B-C-Pt nanoparticles (NPs) were red-shifted to 762 and 985 nm, respectively. The 1O2 quantum yield and photothermal conversion efficiency of the B-C-Pt NPs were 4.0% and 40.6%, respectively. Moreover, B-C-Pt NPs had chemotherapeutic efficacy due to the presence of cisplatin. In vitro and in vivo studies further demonstrated that B-C-Pt NPs had synergistic therapeutic efficacy. Together, B-C-Pt NPs could be employed in NIR Ⅱ fluorescent and photoacoustic imaging-guided synergistic phototherapy and chemotherapy for cancer treatment.
Tuberculosis (TB) is a chronic infectious disease, which is caused by the pathogen Mycobacterium tuberculosis (Mtb) and reemerged as a global health risk with a significant proportion of multi-drug resistant and extensively drug resistant TB cases. It is very urgent to find some novel high-confidence drug targets in Mtb for discovering the effective anti-TB agents. Thioredoxin reductase (TrxR) has been identified to be a highly viable target for anti-TB drugs for its important role in protecting the pathogen from thiol-specific oxidizing stress, regulating intracellular dithiol/disulfide homeostasis and DNA replication and repair. In the present work, a near-infrared (NIR) fluorescent probe DDAT was developed for the detection of TrxR activity and used to high-throughput screen the TrxR inhibitors from natural products. Two screened TrxR inhibitors from Sappan Lignum and microbial metabolites that were further used to inhibit Mycobacterium tuberculosis. All the results indicate that DDAT is a practical fluorescent molecular tool for the discovery of potential anti-TB drugs.
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