Latest ArticlesAs a vital nutrient closely related to the cancer-cells proliferation, phosphate anions have been paid great attention as a promising anticancer agent. Generally, the transport of phosphate anions depends on a protein transport system which is regulated by ion homeostasis regulations. Herein, we designed a reactive anionic nanocarrier based on black phosphorus nanosheets (BPs) and artesunate (ART), which could enter cells through endocytosis to generate phosphate anions, avoiding the regulation of cell homeostasis. The ionic nanocarrier was coated by polydopamine to defend BPs and ART and functionalized by folate (FA) and hyaluronic acid (HA) for targeting factor. With the anchoring groups FA/HA targeted the carrier into cells, polydopamine coating decomposed to expose ART for further generating reactive oxygen species (ROS) in cancer cell microenvironment, providing oxidation conditions. Next, ROS generated by ART makes BPs decompose to phosphate anions with effectively speed, giving rise to the destruction of ion homeostasis to induce necrosis and inhibit the proliferation for cancer cells. In consequence, this research provides novel idea and direction for the ionic carriers and tumor therapeutics.
The design of supramolecular systems with efficient singlet oxygen generation has attracted considerable interests. Herein, an AIE-based singlet oxygen generation system with chemiluminescence properties is reported in aqueous media based on supramolecular host-guest assembly between a water-soluble pillar[5]arene (WP5) and an AIE photosensitizer (TPEDM). The formed supramolecular nanoparticles exhibit significant singlet oxygen generation ability as well as enhanced fluorescence. In addition, by introducing catalase, this H2O2-responsive supramolecular system shows increased 1O2 generation efficiency compared with the blank nanoparticles. An efficient chemiluminescence system can also be achieved by entrapping an energy donor adamantane derivative (AMPPD). Moreover, the present system can function as nanoreactors to perform the photooxidation of dopamine to form polydopamine with visible light irradiation. This work provides a new strategy for the construction of 1O2 generation system based on supramolecular nanomaterials, which has potential applications in the fields such as chemiluminescence imaging and controlled photocatalysis.
Metal organic frameworks (MOFs) derived carbonaceous materials have a wide range of applications in the fields of energy storage, catalysis, adsorption and separation, etc. Especially, zeolitic imidazolate framework-8 (ZIF-8) is an excellent candidate to synthesize porous carbon due to the large surface area and high nitrogen content. However, the dominated microporous structure of ZIF-8-derived carbon significantly hinders ionic mass transfer, limiting the improvement of performance. Herein, MOF-derived mesoporous carbon was prepared using ZIF-8 as carbon precursor and cheap sodium silicate (Na2SiO3) as activator. The introduction of Na2SiO3 created rich mesoporous structure and increased specific surface area, as well as the effects of pyrolysis temperature and Na2SiO3 dosage on performance was also investigated. The obtained ZIF-derived porous carbon exhibits good electrochemical performance with specific capacitance of 263 F/g at 1 A/g and excellent cycle life (96.07% after 10,000 GCD cycles) in supercapacitor. The use of cheap Na2SiO3 activator provides a new orientation for the preparation of MOF-derived carbons with rich pores, high surface area, and facilitates the large-scale application of MOF-derived carbons.
We report a 2-iodoxybenzoic acid (IBX)-mediated intarmolecular oxidative spiro-fused tandem cyclization reaction of tryptophan analogs bearing an N-arylamides side-chain to rapidly afford polycyclic spiroindolines featuring multiple stereocenters including a quaternary stereocenters under mild reaction conditions. Among them, a novelty azaphosphol idine-containing spiroindoline compound is synthesized for the first time. It may open the door to azaphos pholidine-containing spiroindoline compound of potential interest in synthetic and medicinal chemistry. A plausible mechanism is proposed.
A new nonporous Zn-based metal-organic framework (NPMOF) synthesized from a high nitrogen-containing rigid ligand was converted into porous carbon materials by direct carbonization without adding additional carbon sources. A series of NPMOF-derived porous carbons with very high N/O contents (24.1% for NPMOF-700, 20.2% for NPMOF-800, 15.1% for NPMOF-900) were prepared by adjusting the pyrolysis temperatures. The NPMOF-800 fabricated electrode exhibits a high capacitance of 220 F/g and extremely large surface area normalized capacitance of 57.7 μF/cm2 compared to other reported MOF-derived porous carbon electrodes, which could be attributed to the abundant ultramicroporosity and high N/O co-doping. More importantly, symmetric supercapacitor assembled with the MOF-derived carbon manifests prominent stability, i.e., 99.1% capacitance retention after 10,000 cycles at 1.0 A/g. This simple preparation of MOF-derived porous carbon materials not only finds an application direction for a variety of porous or even nonporous MOFs, but also opens a way for the production of porous carbon materials for superior energy storage.
Aphamines A–C (1–3), three pairs of acyclic diterpene dimer enantiomers with an unprecedent ploymerization pattern, were discovered from Aphanamixis polystachya by NMR-guided isolation and chiral resolution. The elucidation of their novel carbon skeletons was achieved based on spectroscopic analysis, exciton chirality, and calculated electronic circular dichroism (ECD). Plausible Claisen rearrangement, 5-exo-trig cyclization, and reduction reactions may play important roles in the polymeric biosynthesis pathway. Compounds 1 and 3 showed inhibitory effects on nitric oxide (NO) production (IC50: 6.71–15.36 μmol/L) and reduced the expression of iNOS in LPS-induced RAW 264.7 macrophages.
A purely organic D-π-A-π-D type emitter showing thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) was designed and synthesized by utilizing the benzophenone as an acceptor and the N-phenyl-2-napthylamine as a donor moiety. It exhibits considerable TADF character in doped PMMA film and room temperature phosphorescence with a long lifetime of 74 ms at 466 nm in solid state. The devices with the configuration of ITO/Mo2O3 (4 nm)/mCP (30 nm)/mCP: x wt% NP2BP/TmTyPB (60 nm)/LiF (1.5 nm)/Al (100 nm) were prepared by vacuum evaporation to explore their electroluminescent performance. Interestingly, the non-doped device has obtained near-white emission with a fluorescence emission peak at 475 nm and a phosphorescence emission peak at 563 nm having the CIE coordinate of (0.23, 0.32) and the maximum external quantum efficiency of 1.09%.
The σ-bond activation by main group element has received enormous attention from theoretical and experimental chemists. Here, the reaction of C–X (X=Cl, Br, Ⅰ) bonds in benzyl and allyl halides with a pincer-type phosphorus(Ⅲ) species was reported. A series of structurally robust phosphorus(Ⅴ) compounds were formed via the formal oxidative addition reactions of C–X bonds to the phosphorus(Ⅲ) center. Density functional theory calculations show that the nucleophilic addition process is more favorable than the direct oxidative addition mechanism. Isomerization of bent structures of phosphorus(Ⅲ) compound to poorly nucleophilic compounds to undergo further C–X bond activation can be rationalized by frontier molecule orbital analysis. This study not only provides a deep understanding of the reactivity of phosphorus(Ⅲ) species but also demonstrates a potential of main group elements for the small-molecule activation.
The catalysts of three-dimensionally ordered macroporous (3DOM) Al2O3-supported core-shell structured Pt@MnOx nanoparticles (3DOM-Pt@MnOx/Al2O3) were successfully prepared by the gas bubbling-assisted membrane reduction-precipitation (GBMR/P) method. Pt@MnOx core-shell nanoparticles (NPs) are highly dispersed on the inner surface of 3DOM-Al2O3 support. Pt@MnOx/3DOM-Al2O3 catalysts, which combine both advantages of high-efficiency soot-catalyst contact by 3DOM-Al2O3 structure and the abundant active sites by the optimized Pt-MnOx interface, exhibit high catalytic activities for soot combustion, and the catalytic activities are strongly dependent on the thickness of MnOx shell. Among the catalysts, 3DOM-Pt@MnOx/Al2O3-1 catalyst with optimized Pt-MnOx interface shows the highest catalytic activity for soot combustion, i.e., its values of T50 and Sm are 351 ℃ and 98.6%, respectively. The highest density of Pt-MnOx active sites for adsorption-activation of gaseous O2 is responsible for enhancing catalytic activity for soot combustion. Pt@MnOx/3DOM-Al2O3 catalysts are promising to practical applications for the emission reduction of soot particles.
Phosphatase plays a vital important role in many biological functions due to the dephosphorylation serves varied roles in cellular regulation and signaling. Among the family of phosphatase, alkaline phosphatase (ALP) could act as crucial prognostic indicators for many diseases such as bone diseases and cancer. However, the detection of ALP is mainly limited to in vitro colorimetric method in clinic. Therefore, huge efforts have been paid on the fluorescence imaging that provides a reliable method to detect the real-time and in vivo changes of the level of ALP. In this review, we summarize recent advances in fluorescence imaging of phosphatase, mainly focused on ALP. The imaging probes of phosphatase are mainly classified according to their luminescence mechanisms. In the end, we assessed the challenges and future prospects of phosphatase probes.
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