Latest ArticlesA new strategy for the metal-free coordination–insertion ring-opening polymerization of tetrahydrofuran by the central metalloid Boron has been first identified. Bis(pentafluorophenyl)(phenoxy)borane was used as a catalyst for the polymerization reaction system. And polytetrahydrofuran with high molecular weight and narrow molecular weight distribution could be obtained. The proposed mechanism was studied by MALDI-TOF, ESI-MS and O-18 isotope labeling analyses as a metal-free coordination insertion mechanism.
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.
LiBr as a promising redox mediator (RM) has been applied in Li-O2 batteries to improve oxygen evolution reaction kinetics and reduce overpotentials. However, the redox shuttle of Br3− can induce the unexpected reactions and thus cause the degradation of LiBr and the corrosion of Li anode, resulting in the poor cyclability and the low round-trip efficiency. Herein, MgBr2 is firstly employed with dual functions for Li-O2 batteries, which can serve as a RM and a SEI film-forming agent. The Br– is beneficial to facilitating the decomposition of Li2O2 and thus decreasing the overpotential. Additionally, a uniform SEI film containing Mg and MgO generates on Li anode surface by the in-situ spontaneous reactions of Mg2+ and Li anode in an O2 environment, which can suppress the redox shuttle of Br3− and improve the interface stability of Li anode and electrolyte. Benefiting from these advantages, the cycle life of Li-O2 battery with MgBr2 electrolyte is significantly extended.
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.
Carbon dots (CDs) have been extensively studied owing to their fascinating optical properties and wide potential applications. Here, we report an easy-to-perform and organic-solvent-free synthesis strategy for green-emissive CDs (G-CDs) possessing high photoluminescence (PL) quantum yield (QY). The G-CDs are synthesized by heating the homogeneous precursors of citric acid and cyanamide in an open vessel, circumventing the use of organic solvents, complex operations, high-pressure reactors, and expensive instruments in the synthesis process. The effect of various reaction variables on the formation and the optical properties of G-CDs are systematically investigated. The resultant G-CDs show bright PL emission at 521 nm with PL QY up to 73%. Then a white light-emitting diode (LED) with Commission Internationable de L'Eclairage (CIE) coordinates of (0.33, 0.34) and color rendering index (CRI) of 92 is constructed based on G-CDs/thermoplastic polyurethane (TPU) composite. Moreover, a visual microfluidic detection platform is designed by using G-CDs as fluorescent probes for rapid quantitative detection of Fe3+, Cu2+, and Mn2+ metal ions, which can realize synchronized testing of multiple samples. This study might promote the development and preparation methods of high-performance CDs with various optical applications.
Here, we report a concise and divergent enantioselective total synthesis of marine sesquiterpene quinone meroterpenoids (+)-dysidavarones A–C (1–3) using predysidavarone 6 as a key common intermediate. The highly strained and bridged eight-membered carbocycle of predysidavarone 6 was constructed by a one-pot intermolecular alkylation and intramolecular arylation of Wieland–Miescher ketone derivative 11 and benzyl bromide 12. The total synthesis of (+)-dysidavarones A–C (1–3) was achieved from predysidavarone 6 in a divergent manner by a late-stage introduction of the ethoxy group, which reveals the possible source of the ethoxy group within (+)-dysidavarones A–C (1–3) and provides a late-stage modifiable route for the synthesis of dysidavarone analogs for further anti-cancer activity evaluation.
The selective electrochemical conversion of glycerol into value-added products is a green and sustainable strategy for the biomass utilization. In this work, Au nanowires (Au-NW) modified with polyethyleneimine (PEI) molecule (Au-NW@PEI) is obtained by an up-bottom post-modification approach. Physical characterization, molecular dynamics simulation and density functional theory demonstrate that the loose-packed PEI monolayer firmly and uniformly distribute on the Au-NW surface due to the strong Au-N interaction. Electrochemical experiments and product analysis display that PEI modification significantly enhance the electro-activity of Au-NW for the glycerol electro-oxidation reaction (GEOR) due to the electronic effect. Meanwhile, the steric hindrance and electrostatic effect of PEI layer make the optimizing adsorption of intermediates possible. Therefore, the selectivity of C3 product glyceric acid over Au-NW@PEI is increased by nearly 20%. The work thus indicates that the rational design of metal-organic interface can effectively elevate the electro-activity and selectivity of Au nanostructures, which may have wide application in biomass development.
Aluminosilicate small pore zeolites belonging to ABC-6 family play crucially important roles in the high methanol conversion with the high selectivity of light olefins, gas separation and storage, and selective catalytic reduction of NOx. In this work, we report a general method, called the epitaxial growth approach, for designing ABC-6 family small pore zeolites. It is mainly realized through the epitaxial growth on the nonporous SOD-type zeolite in the presence of inorganic cations (Na+ and K+) combined with a variety of organic structure directing agents (OSDAs). In this case, a series of ABC-6 family small pore zeolites such as ERI-, SWY-, LEV-, AFX-, and PTT-type zeolites have been successfully synthesized within a few hours. More importantly, the advanced focused ion beam (FIB) and the low-dose high-resolution transmission electron microscopy (HRTEM) imaging technique have been utilized for unraveling the zeolite heterojunction at the atomic level during the epitaxial growth process. It turns out (222) crystallographic planes of the SOD-type zeolite substrate provide unique pre-building units, which facilitate the growth of targeted ABC-6 family small pore zeolites along its c-axis. Moreover, the morphologies of ERI-type zeolite can also be tuned through the epitaxial growth approach, achieving a longer lifetime in the methanol conversion.
A nine cyclic peptide (TCP-1) showed excellent specificity for colon cancer. TCP-1 binds with human tumor tissues at early stages and mice tumor with diameters of 1-4 mm, suggesting that TCP-1 may be used for early diagnosis of colon cancer. The mechanism of the targeted binding of TCP-1 to colon cancer was also studied using immunoprecipitation, LC-MS and bioinformatics. After screening and identifying of the possible binding target proteins of TCP-1, keratin, type Ⅱ cytoskeletal 5 was speculated to be the specific binding target protein of TCP-1 in human tumor tissue. Pharmacokinetics studies were conducted to investigate the target-mediated drug disposition of the new tumor-specific peptide by LC-MS/MS. The tissue distribution study showed that TCP-1 was found only in colon tumors (the target site) in tumor mice did not bind to any other tissues. Conjugating TCP-1 to tumor markedly increased its removal rate from blood circulation but mildly extended its staying time in vivo. In tumor mice, a lower AUC of TCP-1 (reduced by almost 35%) and 2-fold higher clearance were found compared to that of normal mice. The proposed metabolic pathway of TCP-1 in the kidney was also determined using LC-MSn-IT-TOF. The high specificity and low toxicity of the peptide may be caused by its extremely tight binding to the targets. Potential applications for future clinical use, including MRI and PET/CT were also explored, and this research may promote the development of colon cancer diagnostic technology research and provide new ideas and technical routes for tumor diagnostic technology.
Poly(ethylene oxide) (PEO) polymer electrolytes (PEs) have been commercially applied in LiFePO4||Li solid-state lithium batteries (SSLBs). However, it remains challenging to develop PEO-based PEs applicable to the high-voltage SSLBs with higher energy density, owing to the poor electrochemical stability of PEO. Herein, we report a scalable strategy for fabricating PEO-based PEs with high-voltage compatibility, by exploiting a new mechanism to stabilize the cathode-electrolyte interface in the high-voltage SSLBs. The protocol only involves a one-pot synthesis procedure to covalently crosslink the PEO chains, in the presence of high-content lithium bis(trifluoromethylsulphonyl)imide (LiTFSI) salts and N,N-dimethylformamide (DMF). LiTFSI-DMF supramolecular aggregates are formed and firmly embedded in the polymer network, endowing the PE with high room-temperature ionic conductivity. The dissociated and highly concentrated TFSI− anions can enter the Helmholtz layer close to the high-voltage cathode, leading to the formation of a thin and homogeneous cathode electrolyte interface (CEI), mainly composed of LiF, on the cathode. The CEI with high electrochemical stability can effectively stabilize the cathode-electrolyte interface, enabling long-term stable cycling of the high-voltage LiCoO2||Li and nickel-rich NCM622||Li batteries at room temperature. The simplicity and scalability of the strategy makes the reported PEO-based PE potentially applicable in high-voltage SSLBs in practice.
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