Latest ArticlesFabrication of selective adsorption coatings plays a crucial role in solid-phase microextraction (SPME). Herein, new strategies were developed for the in-situ fabrication of novel cobalt-based carbonaceous coatings on the nickel-titanium alloy (NiTi) fiber substrate using ZIF-67 as a precursor and template through the chemical reaction of ZIF-67 with glucose, dopamine (DA) and melamine, respectively. The adsorption performance of the resulting coatings was evaluated using representative aromatic compounds coupled to high-performance liquid chromatography (HPLC) with ultraviolet detection (HPLC-UV). The results clearly demonstrated that the adsorption selectivity was subject to the surface elemental composition of the fiber coatings. The cobalt and nitrogen co-doped carbonaceous coating showed better adsorption selectivity for ultraviolet filters. In contrast, the cobalt-doped carbonaceous coating exhibited higher adsorption selectivity for polycyclic aromatic hydrocarbons. The fabricated fibers present higher mechanical stability and higher adsorption capability for model analytes than the commercial polydimethylsiloxane and polyacrylate fibers. These new strategies will continue to expand the NiTi fibers as versatile fiber substrates for metal-organic frameworks (MOFs)-derived coating materials with controllable nanostructures and tunable properties.
Concentration gradient and fluid shear stress (FSS) for cell microenvironment were investigated through microfluidic technology. The Darcy–Weisbach equation combined with computational fluid dynamics modeling was exploited to design the microfluidic chip, and the FSS distribution on the cell model with varying micro-channels (triangular, conical, and elliptical). The diffusion with the incompressible laminar flow model by solving the time-dependent diffusion–convection equation was applied to simulate the gradient profiles of concentration in the micro-channels. For the study of single cell in-depth, the FSS was investigated by the usage of polystyrene particles and the concentration diffusion distribution was studied by the usage of different colors of dyes. A successful agreement between model simulations and experimental data was obtained. Finally, based on the established method, the communication between individual cells was envisaged and modeled. The developed method provides valuable insights and allows to continuously improve the design of microfluidic devices for the study of single cell, the occurrence and development of tumors, and therapeutic applications.
The urgent need for immediate personal protection against chemical warfare agents (CWAs) spurs the requirement on robust and highly efficient catalytic systems that can be conveniently integrated to wearable devices. Herein, as a new concept for CWA decontamination catalyst design, sub-nanoscale, catalytically active zirconium-oxo molecular clusters are covalently integrated in flexible polymer network as crosslinkers for the full exposure of catalytic sites as well as robust framework structures. The obtained membrane catalysts exhibit high swelling ratio with aqueous content as 84 wt% and therefore, demonstrate quasi-homogeneous catalytic activity toward the rapid hydrolysis of both CWA, soman (GD) (t1/2 = 5.0 min) and CWA simulant, methyl paraoxon (DMNP) (t1/2 = 8.9 min). Meanwhile, due to the covalent nature of cross-linkages and the high flexibility of polymer strands, the membranes possess promising mechanical strength and toughness that can stand the impact of high gas pressures and show high permeation for both CO2 and O2, enabling their extended applications in the field of collective/personal protective materials with body comfort.
Aprotic Li-CO2 batteries have attracted growing interest due to their high theoretical energy density and its ability to use green house gas CO2 for energy storage. However, the poor ability of activating CO2 in organic electrolyte often leads to the premature termination of CO2 reduction reaction (CO2RR) directly. Here in this work, cetyl trimethyl ammonium bromide (CTAB) was introduced into a dimethyl sulfoxide (DMSO) based Li-CO2 battery for the first time to enhance the CO2RR. Significantly improved electrochemical performances, including reduced discharge over-potential and increased discharge capacity, can be achieved with the addition of CTAB. Ab initio molecular dynamics (AIMD) simulations show that quaternary ammonium group CTA+ can accelerate CO2 reduction process by forming more stable contact ion pair (CIP) with CO2-, reducing the energy barrier for CO2RR, thus improving the CO2 reduction process. In addition, adding CTA+ is also favorable for the solution-phase growth of discharge products because of the improved migration ability of stable CTA+-CO2- CIP in the electrolyte, which is beneficial for improving the utilization ratio of cathode. This work could facilitate the development of CO2RR by providing a novel understanding of CO2RR mechanism in organic system.
Silicon (Si) is regarded as the potential anode for lithium-ion batteries (LIBs), due to the remarkable theoretical specific capacity and low voltage plateau. However, the rapid capacity decay resulting from volume variation and slow electron/ion transportation of Si limit its practical application. Here, matryoshka-type carbon-stabilized hollow silicon spheres (Si/C/Si/C) are synthesized by an aluminothermic reduction and calcination process. The Si/C/Si/C anode materials prepared at 500 ℃ (Si/C/Si/C-500) exhibit unique structures, in which amorphous region and porous structure are preserved in the Si layers. The anode based on Si/C/Si/C-500 displays an initial specific capacity of 2792 mAh/g at a current density of 100 mA/g. At 1000 mA/g, this anode retains a reversible capacity of 1673 mAh/g, 86.9% of the initial capacity after 200 cycles. Such synthetic strategy can be employed to fabricate other high-capacity anode materials with large volume variation during charge/discharge process
Selective hydrogenation of substituted nitroarenes is an important reaction to obtain amines. Supported metal catalysts are wildly used in this reaction because the surface structure of supports can tune the properties of the supported metal nanoparticles (NPs) and promote the selectivity to amines. Herein, Pt NPs were immobilized on FeOOH, Fe3O4 and α-Fe2O3 nanorods to synthesize a series of iron compounds supported Pt catalysts by liquid phase reduction method. Chemoselective hydrogenation of 3-nitrostyrene to 3-aminostyrene was used as probe reaction to evaluate the performance of the catalysts. The results show that Pt/FeOOH exhibits the highest selectivity and activity. FeOOH support with pores and -OH groups can tune the electronic structure of Pt NPs. The positive charge of Pt NPs supported on FeOOH is key factor for improving the catalytic performance.
Owing to the exorbitant overpotential and serious carrier recombination of graphitic carbon nitride (g-C3N4), noble metal (NM) is usually served as the H2 evolution co-catalyst. Although the NM (such as Pt) nanoparticles can reduce the H2 evolution overpotential, the weak van der Waals interaction between Pt and g-C3N4 makes against the charge transfer. Herein, the solvothermal method is developed to achieve semi-chemical interaction between Pt and g-C3N4 nanotube (Pt-CNNT) for fast charge transfer. Moreover, the generated in-plane homojunction of CNNT can accelerate charge separation and restrain recombination. Meanwhile, the metallic Pt is an excellent H2 evolution co-catalyst. Photo/electrochemical tests verify that the semi-chemical interaction can improve photogenerated charge separation and transferability of CNNT. As a result, the photocatalytic H2 evolution turnover frequency (TOF) of Pt-CNNT under visible light irradiation reaches up to 918 h−1, which is one of the highest in the g-C3N4-based photocatalysts. This work provides a new idea to improve the charge transfer for efficient photocatalytic H2 evolution.
Neuromuscular blocking agents (NMBAs) are extensively used during anesthesia to improve surgical conditions by relaxing skeletal muscle movements. Rapid neuromuscular recovery after surgery is desirable to facilitate the recovery of muscle function and prevent residual blockade. Decamethonium (C10) is a classic NMBA, which has been restricted over the past decades ascribed to lack of a suitable antidote in clinic. Herein we used carboxylatopillar[6]arene (CP6A) to reverse neuromuscular blocker effect of C10 through direct host-guest encapsulation. NMR and isothermal titration calorimetry served to confirm the complexation between CP6A and C10 with robust affinity [(1.07 ± 0.14) × 107 L/mol]. The CP6A was further used as a reversal agent of C10, which facilitated to decrease C10 concentration in mice blood and excrete via urinary clearance, resulting in rapid recovery from muscle relaxation. These favorable outcomes might lead us to suggest that this supramolecular strategy could allow patients to regain lucidity much faster than spontaneous recovery from anesthesia.
Two-dimensional (2D) covalent organic framework nanosheets (CONs) are attracting increasing research attention because of their unique properties derived from their ultrathin thickness, high surface-to-volume atomic ratio, and extremely large surface area. 2D CONs can provide high transport pathways for charge carriers (e.g., electrons, holes and ions) through either the conjugated skeletons or the open channels. Therefore, they have shown great potential in energy related applications. In this review, we firstly introduce the recent developments and characteristics of 2D CONs by focusing on the two typical synthetic methods, i.e., top-down and bottom-up methods. Then, the energy-related applications in energy storage and conversion of 2D CONs are summarized. Finally, we give our personal views on the challenges and perspectives for the future research of 2D CONs and their composites.
High performance liquid chromatography-mass spectrometry is one of the most commonly used strategies for lipid analysis. The development of versatile chromatographic stationary phases to meet the increasing demands for separation of complex lipids is very important. Styrene-maleic acid (SMA) copolymer is an amphiphilic polymer, which has been proven to have the ability to solubilize lipid molecules of various structures. In this study, styrene-maleic anhydride copolymer coated silica was first prepared by the thiol-ene click reaction. With l-cysteine hydrochloride or dodecanol as the post-modification reagents, Sil-SMA-amino acid and Sil-SMA-dodecanol stationary phase materials were further successfully fabricated via nucleophilic ring-opening reaction. The Fourier-transform infrared, thermogravimetric analysis, and elemental analysis results confirmed the two stationary phase materials were successfully prepared. Furthermore, both the Sil-SMA-dodecanol column and the Sil-SMA-amino acid column possessed reversed-phase/hydrophilic interaction/ion exchange mixed-mode retention mechanisms. The column efficiency of the Sil-SMA-derivatives columns reached 77,300 N/m. Based on the mixed-mode retention characteristics, the Sil-SMA-derivatives columns achieved both the lipid classes and species separation via a single column. The Sil-SMA-amino acid column was further successfully used to separate lipid extract from gastric cancer cell membrane. All these results demonstrated that the SMA-based stationary phase materials have a good potential for use in lipid separation.
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