Latest ArticlesThe 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.
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.
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.
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.
Second near-infrared (NIR-Ⅱ) light triggered in-situ tumor vaccination (ISTV) represents one of the most promising strategies in boosting the whole-body antitumor immunity. While most of previously developed nano-adjuvants for NIR-Ⅱ-triggered ISTV are “all-in-one” formulations, which may indiscriminately damage both the tumor cells and the immune cells, limiting the overall effect of immune response. To overcome this obstacle, we designed a “cocktail” nano-adjuvant by physically mixing hyaluronidases (HAase)-decorated gold nanostars (HA) for NIR-Ⅱ light triggered in situ production of tumor-associated antigens and CpG functionalized gold nanospheres (CA) for immune cells activation. Compared to “all-in-one” formulation, the “cocktail” nano-adjuvants displayed a significantly stronger immune response on NIR-Ⅱ light induced dendritic cells (DCs) mutation and T cells differentiation, greater effect on tumor-growth inhibition, and higher efficacy in inhibition of pulmonary metastases. What is more, increasing the molar ratio of HA to CA led to an enhanced anticancer immune responses. This study highlight the nano-adjuvant formulation effects on the treatment of tumors with multiple targets.
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.
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.
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.
Urea plays a vital role in the sustainable development of mankind as it is one of the most important nitrogen fertilizers. Conventional synthesis of urea is accompanied by a high level of energy consumption while electrocatalytic methods suffer from low yields and poor selectivity. Our work achieves efficient synthesis of urea by designing the graphene-In2O3 electrocatalysts for the co-activated reduction of nitrate and carbon dioxide, where the formation rate of urea, Faraday efficiency (FE) and carbon selectivity at -0.35 V vs. RHE can reach 357.47 µg mg−1 h−1, 10.46% and ~100%, respectively. Herein, the key intermediates in the CN coupling reaction are demonstrated to be *NH2 and *CO2, which is of novelty compared to previous reports. This work may provide inspiration for subsequent studies on the reaction mechanism of the electrochemical synthesis of urea, as well as theoretical guidance for the sustainable synthesis of some other important chemical substances.
Inhibition of mycobacterial membrane protein large 3 (MmpL3) thereby affecting the mycolic acid biosynthetic pathway has been proven to be an effective strategy for developing antitubercular drugs. Based on the X-ray crystal structure of MmpL3 inhibitor complexes, a series of novel 1,2,4-triazole derivatives were designed, synthesized and evaluated antitubercular activity against Mtb strain H37Rv. Comprehensive structure–activity relationship exploration resulted in the identification of compounds 21 and 28, which possess potent antitubercular activity against Mtb strain H37Rv [minimum inhibitory concentration (MIC) = 0.03–0.13 µg/mL] and the clinical isolates of multidrug resistance (MDR) and extensive drug resistance (XDR) tuberculosis (MIC = 0.06–1.0 µg/mL). Moreover, compounds 21 and 28 showed neglectable cytotoxicity (IC50 ≥ 32 µg/mL) to the mammalian Vero cells and favorable physicochemical and pharmacokinetic properties according to the in silico absorption, distribution, metabolism and excretion (ADME) prediction. Finally, the potential target of representative 1,2,4-triazole 28 was identified to be MmpL3 using a microscale thermophoresis (MST) assay.
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