Latest ArticlesMetal nanoparticles (MNPs) possess size-dependent desirable electronic and optical properties while metal-organic frameworks (MOFs) have an edge over extremely large specific surface areas, homogeneous structure, high porosity and remarkable chemical stability. Their combination (MNPs/MOFs) is a novel nanomaterial with broad application prospect in sensing field. To improve performance in sensing applications, we have paid great attention to synergistic effects between the two compositions above. Because of the synergistic effects between MNPs and MOFs, sensors on the basis of MNPs/MOFs composites show significant sensing enhancement with respect to stability, selectivity and sensitivity. In this review, various applications for MNPs/MOFs composites in electrochemical sensing, fluorescent sensing, colorimetric sensing, surface-enhanced Raman scattering sensing and chemiluminescence/electrochemiluminescence sensing are focused and summarized. Besides, the synergistic interactions between MNPs and MOFs was investigated. Finally, based on theoretical information from the reports as well as experimental experience, this review offers the challenges and opportunities for future research on MNPs/MOFs composites.
Hypoxia is a typical characteristic of hepatocellular carcinoma (HCC), which causes tremendous obstacles to tumor treatments. Current first-line treatment may further deteriorate tumor hypoxia. For example, Lenvatinib, a receptor tyrosine kinase inhibitor (RTKI), suppresses tumor growth via blocking vascular endothelial growth factor (VEGF) signaling, and can also inhibit angiogenesis, thus limiting oxygen supply to tumor sites. Therefore, alleviating tumor microenvironment (TME) hypoxia holds great potential for enhancing the therapeutic effect of RTKI. Here, nanoparticle-stabilized oxygen microcapsules, a stable and biocompatible oxygen-loaded delivery system, are successfully prepared through interfacial polymerization of polydopamine nanoparticles. The microcapsules with a large loading capacity of oxygen in the core show excellent bioavailability and dispersity, which could effectively improve the hypoxic TME when they serve as oxygen delivery vehicles. Synergetic treatments of Lenvatinib and oxygen microcapsules could induce the transition of “cold tumor” in an immune-suppressed state to “hot tumor” in an immune-activated state by improving tumor hypoxic TME and reducing angiogenesis in HCC. It is revealed that combined treatments of oxygen microcapsules and Lenvatinib could polarize tumor-associated macrophages (TAMs) to anti-tumor M1 cells and activate T cell-mediated anti-tumor immune responses. The results suggest that synergetic therapy using oxygen microcapsules and Lenvatinib could alleviate the hypoxic TME and enhance the therapeutic performance of RTKI, demonstrating a promising anti-tumor strategy for enhanced therapy of HCC.
A new organocatalytic double annulation cascade involving scission/recombination of N-O bonds of nitrones is reported for the first time, and used to produce a range of hitherto unprecedented tricyclic bridged-fused benzo[d]azepines bearing three stereogenic centers with moderate to good yields and complete diastereoselectivity. A quinine-catalyzed reaction of yne-allenone esters with nitrones worked well and provided a convergent and regioselective pathway to access these three-dimensional scaffolds from the planar conjugated system. Density functional theory (DFT) calculations have been applied to understand the key process for forming diradical intermediates.
A novel method for HDDA-derived benzyne trapped by nitrone was developed. This research described a simple and efficient pathway for the synthesis of benzisoxazoles from arynes and PTIO (2-phenyl-4, 4, 5, 5-tetramethylimidazoline-3-oxide-1-oxyl), C−C and C−O bonds were formed in a single step without catalyst under mild conditions. The unexpected cleavage of C−N bond contributed to the formation of isoxazole ring, as indicated by DFT studies. Furthermore, we obtained the structure of benzoxazolopyrrolidine when the trapping agent is DMPO (5, 5-dimethyl-1-pyrroline N-oxide).
Immune rejection, poor biocompatibility and cytotoxicity have seriously stalled the widespread application of biometallic materials. To overcome these problems, biometallic materials with fast and sufficient osseointegration, antibacterial properties and long-term stability have attracted the attention of researchers worldwide. Surface modification is currently used as a general strategy to develop material coatings that will overcome these challenging requirements and achieve the successful performance of implants. In this study, we proposed a substrate surface-modification strategy based on biofilm CsgA proteins that promote rapid cell attachment, proliferation, and stabilization of the cytoskeleton. CsgA-based nano-coating is easy to fabricate and has superior performance, which is expected to expand the application of medical implants.
30% FeCN/ZIS (30% Fe doped g-C3N4 composited ZnIn2S4) was synthesized by a simple water bath method, via in-situ growth of abundant well-dispersed ZnIn2S4 nanosheets on the Fe doped g-C3N4 surface. Experimental results showed the optimized 30% FeCN/ZIS achieved the best photoreduction of Cr(Ⅵ) performance within a wide pH range, which was 9.5 times and 700 times higher than that of pure ZnIn2S4 and 30% FeCN (Fe doped g-C3N4). This is due to the intense synergy between the Fe-Nx bond and close interface contact produces a high-speed charge transfer channel, thus significantly improving the efficiency of optical carrier separation and migration. Meanwhile, UV-vis diffuse reflection spectra and photoluminescence spectroscopy showed that iron doping significantly narrowed the bandgap of g-C3N4, preventing electron-hole pair recombination. Further, the microstructures and charge separation properties were analyzed by scanning electron microscope, Photoluminescence Spectroscopy and time-resolved photoluminescence, which revealed the structure-activity relationship of composite structure and the synergistic mechanism of each functional component. This research should provide a viable technique for creating composites with high photocatalytic activity for the treatment of chromium-containing wastewater.
Regulating flow direction of photo-excited electrons from interior to active sites in surface is critical to enhance the photocatalytic performance. Herein, photoinduced chemical reduction process was utilized to pinpoint deposit CdS and NiS nanodots sequentially onto g-C3N4 nanosheets. The resulted hybrid composite NiS/CdS/g-C3N4 was much more active under visible light, and eventually boosted the hydrogen evolution rate of 3015 µmol g−1 h−1, to be 2.4 folds better than that of g-C3N4. Because of the relative low content of CdS (around 3.0 wt%), the enhanced activity is due to the favoring band overlapping and promoting charge separation rather than increasing light absorption. Femto-second time-resolved transient absorption spectroscopy (fs-TAS) clearly reveals that the photo-excited electrons are from g-C3N4, and then migrate unidirectionally to CdS and finally to NiS, which is caused by the precisely regulate the position of CdS and NiS on g-C3N4 surface. This study elucidates the electron transfer kinetics and processes in multi-component system and affords a new avenue to construct stable photocatalysts with high activity.
Sulfur mustard (SM) can be absorbed by skin quickly and cause serious system damage via reacting with nearly all cell constituents. Until now, there is still lack of effective antidotal therapy for SM and skin protection is highly important to defend SM. In this article, supramolecular liquid barrier based on pillar[5]arene with triethylene oxide substituents (EGP5) has been designed to impede the skin permeation of SM and further interaction with the skin tissue. EGP5 could encapsulate SM within its cavity, with a Ka value of (5.10 ± 0.47) × 102 L/mol. In vitro skin absorption test proved that EGP5 was capable to effectively prevent SM from penetrating through skin. This supramolecular liquid barrier was employed on rat models to systematically evaluate protective effect against SM intoxication. Pretreatment of EGP5 could alleviate skin and system damage induced by SM and improve survival rate of poisoned rat models from 10% to 90%. Additionally, EGP5 served as protective materials could be highly reused after recycling several times. Overall, these findings have provided the first insight into the construction of convenient liquid material for SM protection.
Metallacycles hold great promise for fluorescence-based sensing due to their synthetic advantages and unique physicochemical properties. However, it remains highly challenging to develop a versatile methodology for constructing highly emissive metallacycles with targeted functionalities and therefore sought-after properties. Herein, we report a general strategy to construct a series of highly emissive perylene diimide-based metallacycles via the self-assembly of perylene diimide-based tetrapyridyl ligand with different dicarboxylic ligands featuring fixed angles and cis-Pt(PEt3)2(OTf)2. Single crystal X-ray diffraction analyses verify the formation of bowtie-like metallacycles with two triangular cavities. Notably, the fluorescence quantum yields of most assemblies exceed 98%, amongst the highest values for metallacycles. Additionally, such metallacycles exhibit sensitive fluorescence responses toward picric acid with a detection limit of 2.8 × 10−6 mol/L. This study not only provides a rational strategy for preparing highly emissive bowtie-shaped metallacycles, but also sheds light on their usage in the detection of picric acid and associated compounds.
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