Latest ArticlesKetones are one of the most important classes of organic compounds, and widely present in various pharmacological compounds, biologically active molecules and functional materials. Over the past few decades, transition metal-catalyzed conversion of aldehydes has been found to be a powerful method. With the continuous development in recent years, it has become an efficient and uncomplicated strategy for constructing ketones. There are four major mechanisms for transition metal-catalyzed ketone synthesis from aldehyde: (1) carbonyl-Heck reaction, that is 1, 2-insertion of organometal species to aldehydic C=O double bond, (2) direct insertion of transition metal catalysts to aldehydic C-H bond, (3) aldehyde as acyl radical, (4) aldehyde as carbon radical acceptor. This article summarizes related reports on the transformations of aldehydes to generate corresponding ketones under different reaction conditions.
H2S selective catalytic oxidation technology is a prospective way for the treatment of low concentration acid gas with simple process operation and low investment. However, undesirable results such as large formation of SO2 and catalyst deactivation inevitably occur, due to the temperature rise of fixed reaction bed caused by the exothermic reaction. Catalyst with high activity in wide operating temperature window, especially in high temperature range, is urgently needed. In this paper, a series of copper-substituted hexaaluminate catalysts (LaCux, x = 0, 0.5, 1, 1.5, 2, 2.5) were prepared and investigated for the H2S selective oxidation reaction at high temperature conditions (300-550℃). The LaCu1 catalyst exhibited excellent catalytic performance and great stability, which was attributed to the best reductive properties and proper pore structure. Besides, two facile deep processing paths were proposed to eliminate the remaining H2S and SO2 in the tail gas.
Formic acid (FA), which can be produced via CO2 reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH2) lead to better catalytic activity compared to that of Pd/KIT-6-NH2 and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h−1 at ambient temperature (303 K), 100% H2 selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH2 can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH2, as well as the amino-groups of KIT-6-NH2 which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.
All-inorganic CsPbI2Br perovskite with suitable bandgap and excellent thermal stability has been reported as the most promising candidate for efficient perovskite solar cells (PSCs). However, the high annealing temperature (> 250 ℃) and poor stability of α-CsPbI2Br greatly limit the future application in photovoltaic field. Herein, a facile method is reported to prepare α-CsPbI2Br perovskite film with high stability at low temperature (70 ℃) by incorporating a small amount of γ-aminobutyric acid (GABA) in the precursor solutions. The devices exhibit reproducible photovoltaic performance with a champion efficiency up to 15.16%, along with the excellent stability, maintaining more than 80% of its initial efficiency after stored in ambient condition for 600 h without any encapsulation. Most importantly, the method enables fabrication of semitransparent CsPbI2Br PSCs with a PCE of 6.76%, as well as an average visible transparency (AVT) of 25.38%. To the best of our knowledge, this is the first attempt to apply CsPbI2Br to the semitransparent solar cells.
Since the outer surface interaction of Q[n]s (OSIQ, including self-, anion- and aromatic-induced OSIQs) was proposed in 2014, it has become the most important research area in our group to construct various Q[n]-based supramolecular frameworks via the OSIQ strategy. Herein, we report a novel supramolecular framework constructed using cucurbit[8]uril (Q[8]) and 4-sulfocalix[6]arene (SC[6]A). This Q[8]/SC[6]A-based supramolecular framework is a product via the perfect combination of self-, anion- and aromatic-induced OSIQs. This framework has the characteristics of easy preparation and high stability with the most important feature being the sequence selective capture of specific metal cations, such as common alkali- and alkaline earth metal ions, and renewability. Thus, this framework may be used in seawater desalination, potassium ion enrichment, radioactive cesium ion pollution source treatment, Gruinard's treatment or water softening and other applications.
An electrochemical sensor (carboxylatopillar[5]arene-coated nitrogen-doped carbon dots, namely CCDs) based on carboxylatopillar[5]arene (CP[5]) functionalized nitrogen-doped carbon dots (N-CDs) has been developed in a facile and economic manner. To improve the performance of this electrochemical sensor in pesticide detection, the optimal solution pH (pH 7) and loading amount of CCDs on the electrode (0.50 mg/mL) have been determined. By virtue of the good conductivity of N-CDs and the molecular recognition property of CP[5], CCDs modified glassy carbon electrode, namely CCDs/GCE, shows excellent anti-interference capability, selectivity, stability, and reproducibility in the sensitive detection of paraquat. The peak currents are proportional to the paraquat concentration (from 0.1 µmol/L to 10 µmol/L) with a detection limit of 6.4 nmol/L (S/N = 3), indicating a great potential in pesticide detection. In comparison with the electrochemical sensors that require expensive metal nanoparticles and complex preparation processes, CCDs/GCE exhibits excellent detection capability of paraquat with lower cost and simpler preparation processes.
Hypoxia is one of the key characteristics of solid tumors. The over-expression of azoreductase resulting from hypoxia can be used as a target to visualize hypoxic levels and a trigger of the drug release system in tumor treatment. In this work, we developed a near-infrared fluorescent probe YLOD, composed of a near-infrared fluorophore, an azo bond, and an analogue of the anti-tumor drug melphalan. In the presence of azoreductase, YLOD displayed a red emission at 620 nm and released the anti-tumor drug concomitantly, thus achieving the integrated effects of hypoxic imaging and tumor treatment. Furthermore, YLOD successfully inhibited the growth of solid tumors during the tumor suppression experiments in nude mice. Considering all the results, YLOD emerges as a new fluorescence tool that can quickly determine the location and the edges of a tumor, showing concrete potential in clinical cancer treatment.
Lignin is the most recalcitrant of the three components of lignocellulosic biomass. The strength and stability of the linkages have long been a great challenge for the degradation and valorization of lignin biomass to obtain bio-fuels and commercial chemicals. Up to now, the selective cleavage of C–O linkages of lignin to afford chemicals contains only C, H and O atoms. Our group has developed a cleavage/cross-coupling strategy for converting 4-O-5 linkage lignin model compounds into high value-added compounds. Herein, we present a palladium-catalyzed cleavage/cross-coupling of the β-O-4 lignin model compounds with amines via dual C–O bond cleavage for the preparation of benzyl amine compounds and phenols.
Pyrazinamide (PZA), isoniazid (INH) and rifampicin (RFP) are all commonly used anti-tuberculosis drugs in clinical practice, and long-term medication may cause severe liver damage and toxicity. The level of peroxynitrite (ONOO–) generated in liver has long been regarded as a biomarker for the prediction and measurement of drug-induced liver injury (DILI). In this article, we constructed a BODIPY-based fluorescent probe (BDP-Py+) that enabled quickly and sensitively detect and image ONOO– in vivo. Utilizing this probe, we demonstrated the change of ONOO– content in cells and mice model of DILI induced by acetaminophen (APAP), and for the first time revealed the mechanism of liver injury induced by antituberculosis drug PZA. Moreover, BDP-Py+ could be applied to screen out and evaluate the hepatotoxicity of different anti-tuberculosis drugs. Comparing with the existing serum enzymes detection and H & E staining, the probe could achieve early diagnosis of DILI before solid lesions in liver via monitoring the up-regulation of ONOO– levels. Collectively, this work will promote the understanding of the pathogenesis of anti-tuberculosis drug induced liver injury (ATB-DILI), and provide a powerful tool for the early diagnosis and treatment of DILI.
Monoamine oxidase A (MAO-A) is a prominent myocardial source of reactive oxygen species (ROS), and its expression and activity are strongly increased in failing hearts. Therefore, accurate evaluation of MAO-A activity in cardiomyocytes is of great importance for understanding its biological functions and early diagnosing the progression of heart failure. However, so far, there is no report on the fluorescent diagnosis of heart failure by a specific probe for MAO-A. In this work, two far-red emissive fluorescent turn-on probes (KXS-M1 and KXS-M2) for the highly selective and sensitive detection of MAO-A were fabricated. Both probes exhibit good response to MAO-A, one of which, KXS-M2, performs better than the other one in terms of a fluorescence increment and sensitivity. Using the pioneering probe KXS-M2, specific fluorescence imaging of MAO-A in glucose-deprived H9c2 cardiac cells, zebrafish and isoprenaline-induced failing heart tissues was achieved, proving that KXS-M2 can serve as a powerful tool for the diagnosis and treatment of heart failure.
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