Latest ArticlesWe herein report a new lanthanide metal-organic framework (MOF) that exhibits excellent chemical stability, especially in the aqueous solution over a wide pH range from 1 to 14. In contrast to many reported lanthanide MOFs, this Tb-based MOF emits cyan fluorescence inherited from the integrated AIE-active ligand, rather than Ln3+ ions. More remarkably, its fluorescence signal features a highly selective and sensitive "turn-off" response toward CrO42−, Cr2O72− and Fe3+ ions, highlighted with the low detection limits down to 68.18, 69.85 and 138.8 ppm, respectively. Thus, the exceptional structural stability and sensing performance render this material able to be a superior luminescent sensor for heavy metal ions in wastewater.
Currently, architecting a rational and efficient nanoplatform combing with multi-therapeutic modalities is highly obligatory for advanced cancer treatment. In order to remedy the self-limiting hypoxic dilemma of photodynamic therapy (PDT), herein, a facile photosensitizer (i.e., chlorin e6, Ce6) and bioreductive prodrug (i.e., tirapazamine, TPZ)-coloaded hyaluronic acid (HA) nanomicelles (denoted as TPZ@HA-Ce6) was developed for the cascading mode of photo-bioreductive cancer therapy. Taking the typical advantage of Ce6 coupled HA conjugate, TPZ was easily and successfully accommodated into the hydrophobic core of HA-Ce6 nanomicelles, yielding TPZ@HA-Ce6. It showed good dispersibility and stability with the hydrodynamic size of ca. 170 nm. It targeted the CD44 overexpressed cancer cells by receptor-mediated endocytosis way and killed them effectively with singlet oxygen and the subsequent TPZ radicals resulting from the oxygen depletion of PDT. The later was further verified by the hypoxia probe in vivo. Using murine mammary carcinoma 4 T1 model, TPZ@HA-Ce6 nanomicelles exhibited cascading and synergistic anticancer effect of PDT and TPZ bioreductive therapy compared with each monotherapy. This work suggests the promising prospect of the hybrid hyaluronic nanomicelles for highly efficient cancer combination treatment.
MicroRNAs are a class of important biomarkers, and the simultaneous detection of multiple miRNAs can provide valuable information about many diseases and biological processes. Amplification-free determination has been developed for the analysis of multiple miRNAs because of its characteristic low cost and high fidelity. Herein, a method for the amplification-free analysis and simultaneous detection of multiple miRNAs based on a so-called pico-HPLC-LIF system is described. In this process, a bare open capillary with an inner diameter of 680 nm is used as a separation column for a sample volume of several hundreds of femtoliters (300 fL), followed by separation and detection. The technique has a zeptomolar limit of detection. The method was applied to detect cellular miRNA from adenocarcinomic human alveolar basal epithelial (A549) cell extracts, and the simultaneous detection of the mir-182, miR-155, and let-7a was achieved. The results showed that the expression of mir-182 and miR-155 was up-regulated and that of let-7a was down-regulated in A549 cells. This method for multiple miRNAs detection is expected to have broad applications in miRNA-based disease diagnosis, prognosis, treatment, and monitoring.
Noble-metal-free photocatalysts with high and stable performance provide an environmentally-friendly and cost-efficient route for green organic synthesis. In this work, CdS nanoparticles with small particle size and different amount were successfully deposited on the surface of covalent organic frameworks (COFs). The deposition of suitable content of CdS on COFs could not only modify the light adsorption ability and the intrinsic electronic properties, but also enhance the photocatalytic activity and cycling performance of CdS for the selective oxidation of aromatic alcohols under visible light. Especially, COF/CdS-3 exhibited the highest yield (97.1%) of benzaldehyde which is approximately 2.5 and 15.9 times as that of parental CdS and COF, respectively. The results show that the combination of CdS and COF can improve the utilization of visible light and the separation of photo-generated charge carriers, and COF with the π-conjugated system as supports for CdS nanoparticles could provide efficient electron transport channels and improve the photocatalytic performance. Therefore, this kind of COF-supported photocatalysts with accelerated photo-induced electrons and charge-carrier separation between semiconductors possesses great potentials in future green organic synthesis.
Lithium metal has a very outstanding theoretical capacity (3860 mAh/g) and is one of the most superior anode materials for high energy density batteries. However, the uncontrollable dendrite growth and the formation of "dead lithium" are the important hidden dangers of short cycle life and low safety. However, the uncontrollable dendrite growth and the formation of dead lithium leads to short cycle life and hidden danger, which hinder its practical application. Controlling the nucleation and growth process of lithium is an effective strategy to inhibit lithium dendrite. Herein, a simple in situ self-catalytic method is used to construct nitrogen doped carbon nanotube arrays on stainless steel mesh (N-CNT@SS) as a lithium composite anode. The N-doped CNTs provide a great number of N-functional groups, which enhance the lithiophilic of anode and provide a large number of uniform nucleation sites, hence it has excellent structural stability for cycles. The arrays provide neat lithium-ion transport channels to uniform lithium-ion flux and inhibits dendrite generation, revealed by the COMSOL multi-physics concentration field simulation. The N-CNT@SS composite anode sustain stable at 98.9% over 300 cycles at 1 mA/cm2. N-CNT@SS as the anode is coupled LiFePO4 (LFP) as the cathode construct a full battery, demonstrating excellent cycling stability with a capacity of 152.33 mAh/g and capacity retaining ratio of 95.4% after 100 cycles at 0.5 C.
The development of low-cost and highly efficient bifunctional electrocatalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of critical importance for clean energy devices such as fuel cells and metal-air batteries. Herein, a sophisticated nanostructure composed of CoS, Co and MoC nanoparticles incorporated in N and S dual-doped porous carbon nanofibers (CoS/Co/MoC-N, S-PCNFs) as a high-efficiency bifunctional electrocatalyst is designed and synthesized via an efficient multi-step strategy. The as-prepared CoS/Co/MoC-N, S-PCNFs exhibit a positive half-wave potential (E1/2) of 0.871 V for ORR and a low overpotential of 289 mV at 10 mA/cm2 for OER, outperforming the non-noble metal-based catalysts reported. Furthermore, the assembled Zn-air battery based on CoS/Co/MoC-N, S-PCNFs delivers an excellent power density (169.1 mW/cm2), a large specific capacity (819.3 mAh/g) and robust durability, demonstrating the great potential of the as-developed bifunctional electrocatalyst in practical applications. This work is expected to inspire the design of advanced bifunctional nonprecious metal-based electrocatalysts for energy storage.
In this paper, the ammonia leaching process and high-energy ball milling method were adapted to recover spent LiCoO2 material. The ammonia reduction leaching mechanism of LiCoO2 material in the ammonia-sodium sulfite-ammonium chloride system was elucidated. Compared with untreated LiCoO2 material, the leaching equilibrium time of LiCoO2 after ball-milled for 5 h was reduced from 48 h to 4 h, and the leaching efficiency of lithium and cobalt was improved from 69.86% and 70.80% to 89.86% and 98.22%, respectively. Importantly, the apparent activation energy and leaching kinetic equation of the reaction was calculated by the shrinking core reaction model, indicating that the reaction was controlled by the chemical reaction.
When treated with an alkoxide base like t-BuOK in aprotic solvent, N-diphenylmethyl imino oxindoles, made conveniently through condensation of corresponding isatins with N-diphenylmethyl amine, are deprotonated to form azaallyl anions. Allylation and alkylation of this type of intermediates proceed smoothly with diverse C-electrophiles. Acidic work up finishes 3-amino-3-allyl/alkyl oxindoles. The overall transformation equals to an umpolung process at the C3 of isatins.
Inflammation is a defense mechanism associated with a wide range of diseases. Celastrol is a small molecule isolated from traditional Chinese medicine with potent anti-inflammation activity. In this study, we established an integrated quantitative proteomics strategy to investigate the acute response to celastrol treatment in a rat macrophage cell line challenged with lipopolysaccharide (LPS). Both stable-isotopic based non-targeted quantitative profiling and PRM-based targeted quantitation methods were employed. Dimethyl-labeling based non-targeted profiling revealed 28 and 52 proteins that significantly up- and down-regulated by celastrol. Bioinformatics analysis pinpoint key signaling pathways affected. Seven proteins were selected for examining their time-dependent regulatory pattern in response to celastrol using targeted PRM quantitation. The abundance of mRNA at multiple time-points of selected proteins was also examined. Celastrol induced an acute response of selected key transcriptional factors in terms of mRNA or protein abundance within one hour. Interestingly, regulatory trend of mRNA and protein abundance suggested a novel dual mechanism of celastrol in the terms of acute anti-inflammation. The integrated quantitative proteomic strategy established in this study constitutes an efficient workflow to characterize key components and their time-dependent regulatory pattern for monitoring drug response.
Chiral α-substituted 1, 3-dihydroisobenzofurans are key scaffolds in a number of bioactive natural products and synthetic pharmaceuticals. However, catalytic asymmetric approaches have been rarely developed. Here, a redox deracemization technology is adopted to address the catalytic asymmetric synthesis. A broad range of α-aryl substituted 1, 3-dihydroisobenzofurans are effectively deracemized in high efficiency with excellent ee. α-Alkynyl substituted ethers were also compatible with the deracemization technology.
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