Latest ArticlesAs 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.
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.
Two 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.
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.
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.
Polymerase chain reactions (PCR) are a very important tool for use in cloning, nucleic acid sequencing and diagnostic testing. The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are needed. In this paper, we report using metal ions to form coordination nanomaterials with the intrinsic components of the PCR reagents including dNTP, DNA primers and DNA polymerase as an integrated PCR reaction system. To complete PCR reactions, users need only to dissolve the coordination nanomaterials with a buffer and add template DNA. A few transition metal ions were screened and Cu2+ was found to be the most effective metal ion for this purpose. Then the encapsulation efficiency of PCR reagents was measured, which can reach close to 100% for the primers and DNA polymerase, but only 10% for dNTP because dNTP was excess. Further study also exhibited this integrated PCR reaction system can be used for DNA detection with a similar detection limit to the normal PCR, and showed good stability of encapsulated PCR nanomaterial after storage for a week.
Plasmonic metal nanomaterials with intrinsic surface–enhanced Raman scattering (SERS) and photothermal properties, especially AuAg nanoalloys with both the outstanding merits of Au and Ag nanocrystals, show huge application prospects in bacterial theranostics. However, the direct exposure of AuAg nanoalloys in external conditions probably cause undesirable reactions and poisonous metal ion leakage during SERS detection and photothermal antibacterial therapy process, which severely hinder bacterial theranostics applications. Herein, we report an ultrastable graphene–isolated AuAg nanoalloy (GAA) with AuAg core confined in few–layer graphitic shell as a versatile platform for bacterial detection and therapy. The encapsulation of graphene ensures the good stability of AuAg core, that its superior SERS and photothermal properties are therefore further guaranteed. GAA is used for SERS detection of two vital bacterial biomarkers (including corrosive cyanide and pyocyanin), exhibiting good SERS quantitative and multiplexing ability. GAA is further used for photothermal antibacterial therapy application, and ultrahigh antibacterial efficacies for both Gram–negative Escherichia coli and Gram–positive Staphylococcus aureus are achieved under 808 nm laser irradiation. This work proposes a valuable method to develop robust bacterial theranostic platform.
Available online Immunoglobulins G (IgGs) are Y-shaped globular proteins, however, their high flexibility and heterogeneity pose great challenges to their structure and conformation determinations. Geometric structure of IgG closely correlates to its biofunctions, such as the antibody escape of human immunodeficiency virus (HIV) could attribute to the distance mismatch between the ends of two Fab arms (antigen-binding sites) and envelope glycoprotein spikes on virion surface. Herein, we report the first use of mobility capillary electrophoresis (MCE) and native mass spectrometry (nMS) to resolve the internal geometric structure and conformation of an IgG (trastuzumab) in solution phase. After proteolysis, the ellipsoid dimensions of IgG and its subunits were measured by MCE-nMS experiments. IgG was then reconstructed, in which the sizes and relative positions of these three subunits in three-dimensional space were characterized. It was found that the two Fab arms have an angle of ~102.1° and a distance of ~11.0 nm between the two antigen-binding sites under native condition, and the Fc arm was tilted ~16.0° towards one of the Fab arms. Fc was not on the plane of Fab-Fab, but has an angle of no larger than 103.1°. Under acidic environment (pH 3.0), each subunit of the IgG would unfold into larger dimensions, and the angles between these subunits also change. With great potential for tumor imaging and therapy, the structure of F(ab′)2 fragments was also measured and validated by molecular dynamic simulation. It was found that the electrostatic force among these three subunits and steric hindrance stemming from Fc help maintaining the angle between two Fab arms.
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