Latest ArticlesOptical thermometry as an important local temperature-sensing technique, has received increasing attention in scientific and industrial areas. However, it is still a big challenge to develop luminescent materials with self-activated dual-wavelength emissions toward high-sensitivity optical thermometers. Herein, a novel ratiometric thermometric strategy of Bi3+-activated dual-wavelength emission band was realized in the same lattice position with two local electronic states of La3Sb1-xTaxO7:Bi3+(0 ≤ x ≤ 1.0) materials based on the different temperature-dependent emission behaviors, benefiting from the highly-sensitive and regulable emission to the coordination environment of Bi3+. The structural and spectral results demonstrate that the emission tremendously shifted from green to blue with 68 nm and the intensity was enhanced 2.6 times. Especially, the visual dual-wavelength emitting from two emission centers was presented by increasing the Ta5+substitution concentration to 20% or 25%, mainly originating from the two local electronic states around the Bi3+ emission center. Significantly, the dual-wavelength with different thermal-quenching performance provided high-temperature sensitivity and good discrimination signals for optical thermometry in the range between 303 and 493 K. The maximum relative sensitivity reached 2.64%/K (La3Sb0.8Ta0.2O7:0.04Bi3+@383 K) and 1.91%/K (La3Sb0.75Ta0.25O7:0.04Bi3+@388 K). This work reveals a rational design strategy of different local electronic states around the single-doping multiple emission centers towards practical applications, such as luminescence thermometry and white LED lighting.
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.
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.
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.
Highly efficient catalysts for electrolysis of water are crucial to the development of hydrogen energy which is helpful to carbon neutralization. Recently, high temperature shock (HTS), with advantage of rapid speed, universality and scalable production, has been a promising method in synthesis of nanomaterials. In this paper, HST was used to treat low Pt loading Mo6S8 for enhanced water splitting performance. Impressively, the optimized MoS2/MoO2/Mo6S8 nano-composite with low Pt mass loading (~4%) displays well hydrogen evolution reaction (HER) electrochemical performance. The overpotential is 124 mV to reach 10 mA/cm2 and the corresponding Tafel slope is 88 mV/dec in acidic electrolyte. Its mass activity is 6.2 mA/µgPt at -124 mV vs. RHE, which is almost 2 times relative to 20% Pt/C. Moreover, it presents distinguished stability even after 2000 cycles. This work will broaden the way of catalysts preparation and the application of hydrogen evolution.
Bare Pd metal nanoparticles invariably suffer from poor selectivity in furfural hydrogenation by forming flat configurations, with the aromatic ring of the substrate molecules parallel to the metal surface. Herein, we put forward a promising solution by using CeO2 as promoters to modify Pd nanoparticles for modulating the adsorption behaviors of furfural molecules. To achieve the highly-desired ultra-small Pd@CeO2 core@shell nanostructure, a "constrained auto-redox" synthesis is developed, in which silicalite-1 supports play the key role of providing their surface as the landing place of PdOx precursors for inhibiting the overgrowth and the deformation. To the best of our knowledge, this is one of the smallest core@shell materials obtained from aqueous synthesis. When evaluated as catalysts, Pd@CeO2/S-1 gives 98.9% conversion of furfural with 94.3% selectivity for furfural alcohol in 15 h, which is much better than that of Pd/S-1 (88.6% conversion with 44.3% selectively). The DFT simulation reveals a strong interaction between the defects of CeO2 and the oxygen atom of the –CHO group in furfural molecules, which benefits the selective hydrogenation occurred in the –CHO group rather than the furan ring.
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.
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.
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.
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.
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