Latest ArticlesThe electrochemical CO2 reduction reaction (CO2ER) is an emerging process that involves utilizing CO2 to produce valuable chemicals and fuels by consuming excess electricity from renewable sources. Recently, Cu and Cu-based nanoparticles, as earth-abundant and economical metal sources, have been attracting significant interest. The chemical and physical properties of Cu-based nanoparticles are modified by different strategies, and CO2 can be converted into multicarbon products. Among various Cu-based nanoparticles, Cu-based metal-organic frameworks (MOFs) are gaining increasing interest in the field of catalysis because of their textural, topological, and electrocatalytic properties. In this minireview, we summarized and highlighted the main achievements in the research on Cu-based MOFs and their advantages in the CO2ER as electrocatalysts, supports, or precursors.
Through-space charge transfer (TSCT) is regarded as an effective way to develop thermally activated delayed fluorescence (TADF) emitters. Based on this strategy, many molecular frameworks have been proposed, among which spirobased scaffolds have been extensively studied due to their unique advantages. In this work, we developed three emitters SPS, SPO, and SPON, which were constructed with the same donor and various acceptors to explore the influence of acceptor modulation at the C9 position of fluorene for spirostructure TSCT emitters. The results show that the acceptor with too weak electron-withdrawing ability will cause the emitter to not have TADF properties, while the acceptor with too much steric hindrance will weaken the face-to-face π-π stacking interaction between donor/acceptor (D/A). Since SPO balances the electron-withdrawing strength and steric hindrance of the acceptor, it achieves the highest external quantum efficiency (EQE) of 17.75%. This work shows that appropriate acceptor selection is essential for the TADF properties and high efficiency of the spirobased scaffold TSCT emitter
Two bis-naphthalimide-based supramolecular gelators (NN-3 and NN-4) with a little difference of position of amino groups were designed and synthesized for the detection of oxaloyl chloride and phosgene. Energy transfer could be occurred between two naphthalimide groups in molecules NN-3 and NN-4. Yellow gels NN-3 and NN-4 were formed in some mixed solvents, and nanofibers with different size were obtained in these gels. The self-assembly processes of NN-3 and NN-4 in different solvents were investigated by UV-vis absorption, fluorescent spectra, SEM, FTIR, XRD and NMR. Gelators NN-3 and NN-4 could selectively detect oxaloyl chloride in solution and film states, but detect phosgene only in solution. NN-3 exhibited the ratiometric detection ability towards oxaloyl chloride and phosgene with the low limit of detection (LOD) of 210 nmol/L and 90 nmol/L, respectively. NN-4 as the corresponding control sample, it owned the higher LOD towards oxaloyl chloride and phosgene of 12.4 µmol/L and 64 µmol/L, respectively. Interestingly, films NN-3 and NN-4 could sensitively detect oxaloyl chloride gases with the low LOD of 2.0 ppm and 8.34 ppm, respectively. The detection mechanisms of NN-3 and NN-4 were well studied by 1H NMR titration, HRMS and theoretical calculation.
Zinc-ion batteries are under current research focus because of their uniqueness in low cost and high safety. However, the pursuing of high-performance cathode materials of aqueous Zinc ion batteries (AZBs) with low cost, high energy density and long cycle life has become the key problem to be solved. Herein we synthesized a series of amorphous nickel borate (AM-NiBO) nanosheets by varying corrosion time with in-situ electrochemical corrosion method. The AM-NiBO-T13 as electrode material possesses a high areal capacity of 0.65 mAh/cm2 with the capacity retention of 95.1% after 2000 cycles. In addition, the assembled AM-NiBO-T13//Zn provides high energy density (0.77 mWh/cm2 at 1.76 mW/cm2). The high areal capacity and better cycling performance can be owing to the amorphous nanosheets structure and the stable coordination characteristics of boron and oxygen in borate materials. It shows that amorphous nickel borate nanosheets have great prospects in the field of energy storage.
Single atom catalysts (SACs) with atomically dispersed transition metals on nitrogen-doped carbon supports have recently emerged as highly active non-noble metal electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), showing great application potential in Zn-air batteries. However, because of the complex structure-performance relationships of carbon-based SACs in the oxygen electrocatalytic reactions, the contribution of different metal atoms to the catalytic activity of SACs in Zn-air batteries still remains ambiguous. In this study, SACs with atomically dispersed transition metals on nitrogen-doped graphene sheets (M-N@Gs, M = Co, Fe and Ni), featured with similar physicochemical properties and M-N@C configurations, are obtained. By comparing the on-set potentials and the maximum current, we observed that the ORR activity is in the order of Co-N@G > Fe-N@G > Ni-N@G, while the OER activity is in the order of Co-N@G > Ni-N@G > Fe-N@G. The Zn-air batteries with Co-N@G as the air cathode catalysts outperform those with the Fe-N@G and Ni-N@G. This is due to the accelerated charge transfer between Co-N@C active sites and the oxygen-containing reactants. This study could improve our understanding of the design of more efficient bifunctional electrocatalysts for Zn-air batteries at the atomic level.
Inhibiting the side reactions while promoting hydrogenation are the main target for the production of functional anilines from nitroarenes; consequently, the preparation of an ideal catalyst to improve chemical selectivity is one of the hot issues. In this work, we provided an easy-to-prepare catalyst with N-doped carbon layers, where the FexOy nanoparticles were encapsulated and distributed uniformly. The structural features of catalyst were characterized by several techniques, and the selected catalyst was next applied to the hydrogenation of nitrobenzene under varied conditions, involving temperature, holding period and H2 pressure. Subsequently, we conducted the synthesis of more than 16 substrates for the corresponding anilines with varied functional groups. The hydrogenation protocol to gram-scale synthesis as well as lifecycle performance were also demonstrated in the batch reactor, together with the explanation of its catalytic mechanisms. Overall, the present work provides an available preparation of simple but highly efficient catalysts for the production or aromatic amines, which will be benefit for the sustainable development of this field in near future.
Herein, an intense electrochemiluminescence (ECL) was achieved based on Pt hollow nanospheres/rubrene nanoleaves (Pt HNSs/Rub NLs) without the addition of any coreactant, which was employed for ultrasensitive detection of carcinoembryonic antigen (CEA) coupled with an M-shaped DNA walker (M-DNA walker) as signal switch. Specifically, in comparison with platinum nanoparticles (Pt NPs), Pt HNSs revealed excellent catalytic performance and pore confinement-enhanced ECL, which could significantly amplify ECL intensity of Rub NLs/dissolved O2 (DO) binary system. Then, the tracks and M-DNA walker were confined on the Pt HNSs simultaneously to promote the reaction efficiency, whose M-structure boosted the interaction sites between walking strands and tracks and reduced the rigidity of their recognition. Once the CEA approached the sensing interface, the M-DNA walker was activated based on highly specific aptamer recognition to recover ECL intensity with the assistance of exonuclease Ⅲ (Exo Ⅲ). As proof of concept, the "on-off-on" switch aptasensor was constructed for CEA detection with a low detection limit of 0.20 fg/mL. The principle of the constructed ECL aptasensor also enables a universal platform for sensitive detection of other tumor markers.
Bacterial antimicrobial resistance (AMR) is a severe threat to global health and development. Under the stimulation of antibiotics, bacterial cells can undergo filamentation and generate daughter cells with stronger AMR. The current research on bacterial AMR mechanism is mainly conducted with a population of cells. However, bacterial cells exhibit heteroresistance, making the study at population level not reliable. Herein, we developed single bacterial cell metabolic profiling by mass spectrometry (MS) to study bacterial AMR at single-cell level. By utilizing a microprobe controlled by a microoperation platform, single filamentous extended spectrum beta-lactamase (ESBL) producing Escherichia coli (ESBL-E. coli) cells generated by ceftriaxone sodium stimulation can be extracted and spray-ionized for MS analysis. Heterogeneous among ESBL-E. coli cells under the same antibiotic stimulus condition was observed from mass spectra as well as cell morphology. The metabolic profiles by MS of different individual cells can be clustered into subgroups well in accordance with bacterial cell length. Metabolic pathways including arginine and proline metabolism, as well as cysteine and methionine metabolism were disclosed to play an important role in the bacterial SOS-associated filamentation against antibiotics. The microprobe electrospray ionization-MS-based single bacterial cell analysis method is promising in the study of various bacterial AMR mechanism and can reveal the heterogeneity of bacterial AMR from-cell-to-cell.
As one of the top global health problems, the effective treatment of cancer is one of the most urgent clinical challenges. Currently, the main treatments for cancer include surgery, chemotherapy, radiotherapy, and gene therapy etc. Chemotherapy is one of the most commonly used treatments, however it has limitations such as highly toxic side effects and low drug utilization rate that limit its application. Gene therapy, as an emerging cancer treatment, has limitations such as drug instability, off-target effects and low internalization efficiency. Poly(amino acid)s carriers with good biocompatibility, degradability and multifunctionality as drug carriers have received much attention, as they can reduce the toxic side effects of chemotherapy, improve drug utilization, and enhance the internalization efficiency and utilization of gene drugs. However, little attention has been paid to the nature of the carriers themselves. This paper reviews the immunomodulatory, anti-inflammatory, antioxidant, internalization-promoting and apoptosis-promoting functions of poly(amino acid)s drug carriers in tumor therapy to provide a theoretical basis for different carrier-drug-adapted synergistic therapies.
The Ni−Al bimetallic catalysis of intramolecular enantioselective and regioselective C−H cyclization of 4-oxoquinazolines with tethered alkenes has been successfully developed. Some new secondary phosphine oxides (SPOs) with large steric hindrance (SPO6-11) were designed and successfully synthesized from readily available chiral amines or amino acids. The developed chiral SPOs as ligands or preligands demonstrate much higher efficiency in the asymmetric catalytic reactions than the reported traditional ones. A new class of chiral tricyclic pyrroloquinazolinones were obtained in up to 95% yield and 99% ee.
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