Latest ArticlesSelective separation of CO2/CH4 and C2H2/CH4 are promising for their high-purity industrial demand and scientific research on account of the similar molecular radius and physical properties. In this work, a unique 3D microporous MOF material [Cu(SiF6)(sdi)2] solvents (1, sdi = 1, 1'-sulfonyldiimidazole) was successfully constructed by cross-linking 1D coordination polymer chains. The dense functional active sites on the inner walls of the channel of 1a can provide strong binding affinities to CO2, C2H2, and thus effectively improve the gas separation performance of CO2/CH4 and C2H2/CH4.
Here, the selective adsorption behaviors of guest molecule COR in two hexamer host grids were investigated by means of scanning tunnelling microscope (STM). The assembled structures of small functional organic molecules TTBTA and TATBA were thermodynamically stable. Interestingly, the introduction of the guest molecule COR destroyed the original hexamer structure of TTBTA and combined with it to form a new triangular host-guest system. Different from TTBTA, the introduction of the guest molecule COR did not affect the six-membered ring structure of TATBA. Furthermore, the co-assembly structure of TTBTA/TATBA/COR was established and the guest molecule COR showed preferential adsorption to the TATBA host grid. Density functional theory (DFT) calculations had been performed to disclose the mechanism of the involved assemblies.
Using the global particle-swarm optimization method and density functional theory, we predict a new stable two-dimensional layered material: MgSiP2 with a low-buckled honeycomb lattice. Our HSE06 calculation shows that MgSiP2 is an indirect-gap semiconductor with a band-gap of 1.20 eV, closed to that of bulk silicon. More remarkably, MgSiP2 exhibits worthwhile anisotropy along with electron and hole carrier mobility. A ultrahigh electron mobility is even up to 1.29×104 cm2 V-1 s-1, while the hole mobility is nearly zero along the a direction. The large difference of the mobility between electron and hole together with the suitable band-gap suggest that MgSiP2 may be a good candidate for solar cell or photochemical catalysis material. Furthermore, we explore MgSiP2 as an anode for sodium-ion batteries. Upon Na adsorption, the semiconducting MgSiP2 transforms to a metallic state, ensuring good electrical conductivity. A maximum theoretical capacity of 1406 mAh/g, a small volume change (within 9.5%), a small diffusion barrier (~0.16 eV) and low average open-circuit voltages (~0.15 V) were found for MgSiP2 as an anode for sodium-ion batteries. These results are helpful to deepen the understanding of MgSiP2 as a nanoelectronic device and a potential anode for Na-ion batteries.
Structure-efficacy effect of small molecular drug attracts wide attentions, but it has always been ignored in nanomedicine research. To reveal the efficacy modulation of nanomedicine, we developed a new type of paclitaxel (PTX)-conjugated gold nanoparticles (PTX-conjugated GNPs) to investigate the influence of drug position in controlling their in vitro properties and in vivo performance. Two therapeutic ligands (TA-PEG-NH-N=PTX and TA-PTX=N-NH-PEG) were synthesized to conjugate PTX on the surface of GNPs at different positions, locating on the surface of gold conjugate and inserting between GNPs and polyethylene glycol (PEG, molecular weight 1000 Da), respectively. It was found that PEG-PTX@GNPs with PTX located between GNP and PEG exhibited higher aqueous solubility, biocompatibility, and stability. In addition, an acid sensitive hydrazone bond has been inserted between PTX and PEG in both ligands for drug release of PTX and PTX-PEG segment, respectively, at the tumor site. Further release of PTX from PTX-PEG segment is based on the esterase hydrolysis of an ester bond between PTX and PEG. This two-step drug release mechanism offers PEG-PTX@GNPs effective and sustained release behavior for desirable anticancer activity, enhanced therapeutic efficacy, and lower systematic toxicity in Heps-bearing animal models.
Photoelectrochemical (PEC) water splitting is a promising approach for renewable hydrogen production. However, the practical PEC solar-to-fuel conversion efficiency is still low owing to poor light absorption and rapid recombination of charge carriers in photoelectrode. In this work, we report a ternary photoanode with simultaneously enhancement of light absorption and water oxidation efficiency by introducing copper phthalocyanine (CuPc) and nickel iron-layered double hydroxide (NiFe-LDH) on TiO2 (denoted as TiO2/CuPc/NiFe-LDH). An experimental study reveals that CuPc loading on TiO2 bring strong visible light absorption; NiFe-LDH as an oxygen evolution reaction catalyst efficiently accelerates the surface water oxidation reaction. This synergistic effect of CuPc and NiFe-LDH gives enhanced photocurrent density (2.10 mA/cm2 at 0.6 V vs. SCE) and excellent stability in the ternary TiO2/CuPc/NiFeLDH photoanode.
The potassium-ion batteries (PIBs) have become the promising energy storage devices due to their relatively moderate cost and plenteous potassium resources. Whereas, the main drawback of PIBs is unsatisfactory electrochemical performance induced by the larger ionic radius of potassium ion. Herein, we report a well-designed, uniform-dispersed, and morphology-controllable zinc sulfide (ZnS) quantum dots loading on graphene as an anode in the PIBs. The directed uniform dispersion of the in-situ growing ZnS quantum dots (~2.8 nm in size) on graphene can mitigate the volume effect during the insertion-extraction process and shorten the migration path of potassium ions. As a result, the battery exhibits superior cycling stability (350.4 mAh/g over 200 cycles at 0.1 A/g) and rate performance (98.8 mAh/g at 2.0 A/g). We believe the design of active material with quantum dot-minimized size provides a novel route into PIBs and contributes to eliminating the major electrode failure issues of the system.
Most recently, cobalt sulfide (CoS) nanospheres (NSs) have been demonstrated as an ideal high-efficient photothermal agent for tumor elimination. However, the surface of CoS NSs is lack of functional chemical groups or active radicals to incorporate therapeutic agents, which tremendously hinders their versatile utilization in medical field. Here, surface activation of CoS NSs was realized through the growth of polydopamine (PDA) in situ via alkaline-triggered polymerization. Upon the formation of CoS@PDA NSs, thiol-polyethylene glycol (SH-PEG) and chemotherapeutic agent of doxorubicin (DOX) were loaded onto the particle surface by means of π-π electrostatic interaction and Michael addition reactions. As-synthesized CoS@PDA/PEG/DOX (CoPPD) NSs exhibited an admirable photothermal property and high loading capacity of DOX (44.6%). Furthermore, drug release can be accelerated under a more acidic pH condition mimicking tumor microenvironment (TME), ascribed to the protonation of amino group in DOX molecules. Finally, a strong chemotherapeutic-enhanced photothermal therapeutic effect was demonstrated toward solid tumor under near-infrared (NIR) light irradiation without causing significant systemic toxicity. In this regard, this paradigm may offer valuable guidance for the design of multifunctional CoS-based nanoagents for medical treatment.
Multishelled hollow structures have drawn increasing interest because of their peculiar compartmentation environments and physicochemical properties. In this work, deformable double-shelled hollow mesoporous organosilica nanocapsules (DDHMONs) were successfully synthesized by a multi-interfacial etching strategy. The obtained DDHMONs have a double-shelled structure with aninorganic-organic hybrid framework, a uniform outer layer (~320 nm) and inner layer (~180 nm), ordered mesochannels (~2.21 nm), and a large specific surface area (~1233 m2/g). In vitro toxicity tests show that the DDHMONs have excellent biocompatibility when coincubated with human breast cancer cells. In addition, the anticancer substance doxorubicin (DOX) can be highly loaded in DDHMONs (~335 μg/mg). The results from flow cytometry together with confocal laser scanning microscopy show that DOX can be efficiently delivered into MCF-7 cells by DDHMONs, thus improving chemotherapeutic efficiency and demonstrating that DDHMONs have potential nanomedicine applications as anticancer agents.
An electrochemical amino-azidation of 2-aminostyrene with sodium azide (NaN3) was developed, which can be carried out smoothly in water under metal-free condition, affording a series of 3-azido indolines with high yields.
Size-controlled flow synthesis of nanoporous particles are of considerable interest for future industrial applications, however, is facing challenges due to lack of in-situ method for size-characterization in fluidic environment. We present that ultraviolet-visible (UV–vis) absorption spectroscopy can be integrated into a flow-synthesis system which was produced by femtosecond laser micromachining. The shift of the absorption peak position of the ex-situ and in-situ UV–vis spectra correlates to variation of size of porous metal-organic frameworks crystals. ZIF-67 crystals with a size in the range from 200 nm to 1025 nm are fabricated with the assistance of tri-ethylamine under monitoring of in-situ UV–vis spectra. The ZIF-67 crystals are converted into nanoporous carbons particles with controlled sizes. These materials show size-dependent performance in Na-ion battery and size-independent performance in metal/H2O seawater battery.
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