Latest ArticlesAn unexpected in-situ hydrolysis reaction occurred during the solvothermal reaction of N, N'-bis(4-carboxy-2-methylphenyl)pyromellitic di-imide) and Ba(NO3)2, and a novel porous Ba-MOF, [H2N(CH3)2]0.5[Ba1.5(L)(DMA)]·1.5DMA·1.5H2O (UPC-70, H3L = 2-(4-carboxy-2-methylphenyl)-1, 3-dioxoisoin-doline-5, 6-dicarboxylic acid, DMA = N, N-dimethylacetamide), was obtained on the basis of the partial hydrolysate. The as-synthesized 3D network with 1D open channels of different sizes (24 Å and 10 Å) contains abundant open metal sites after removal of solvents, which is conducive to the preferential adsorption of CO2. The subsequent gas sorption measurement reveals the high separation selectivity of UPC-70 for CO2/CH4 (15) and CO2/N2 (32) at ambient conditions, and GCMC theoretical simulation provides good verification of the experimental results, indicating that UPC-70 is a potential candidate for CO2 capture from flue gas and natural gas.
Three novel polycyclic polyprenyled acylphloroglucinols, Hyperscabins A-C, were obtained from the aerial parts of Hypericum scabrum. They featured an unprecedented 5, 5-spiroketal subunit with the loss of C-2' carbonyl in the phloroglucinol ring. Their structures were characterized by extensive spectroscopic analyses, NMR calculations with DP4+ analysis, calculated electronic circular dichroism (ECD) spectra and the application of modified Mosher's methods. In the assay of [3H]-5-HT and [3H]-NE reuptake inhibition, compounds 1 and 2 showed good inhibitory activity (81.8% and 83.2%) in 10 μmol/L. In addition, compound 1 significantly increased cell viability in the experiment of oxygen and glucose deprivation/deoxygenation.
The development of a practical synthetic method to functionalize hollow mesoporous silica with organic groups is of current interest for selective adsorption and energy storage applications. Herein, a facile and controllable one-pot approach for the synthesis of monodisperse amino-functionalized hollow mesoporous silica nanoparticles is presented. A novel solid-to-hollow structural transformation procedure of the silica nanoparticles is presented. The structural transformation is easily designed, as observed through transmission electron microscopy, by tailoring the HCl and N-lauroylsarcosine sodium molar ratio and the water content in the sol-gel. Ordered and radially oriented in situ amino-functionalized mesochannels were successfully introduced into the shells of the hollow silica nanoparticles. A formation mechanism for the hollow mesoporous silica materials is discussed.
Non-enzymatic electrochemical sensors for the determination of hydrogen peroxide (H2O2) have attracted more and more concerns. A series of nickel and cobalt double oxides (NixCoy-DO) with the different ratios of Ni/Co have been prepared by a polyol-mediated solvothermal method for H2O2 detection. The obtained products exhibit honeycomb-like open porous microtubes constituted with the low-dimensional nanostructured NixCoy-DO blocks after the calcination treatment. Compared with nickel oxides, the introduced Co ions in NixCoy-DO can induce the production of surficial oxygen vacancies, and further enhance the electrode surface activity. In particular, the NiCo-DO sample (with an atomic ratio of Ni/Co = 4:3) shows the richest surficial oxygen vacancies and presents the highest H2O2 detection activity among all the as-prepared samples, demonstrating an excellent sensitivity of 698.60 μA L mmol-1 cm-2 (0 ~ 0.4 mmol/L), low detection limit (0.28 μmol/L, S/N = 3), as well as long stability, high selectivity and good reproducibility. This work lends a new impetus to the potential application of double metal oxides for the next generation of non-enzymatic sensors.
Catalytic transfer hydrogenation (CTH) of furfural (FF) to furfuryl alcohol (FFA) has received great interest in recent years. Herein, Cu-Cs bimetallic supported catalyst, CuCs(2)-MCM, was developed for the CTH of FF to FFA using formic as hydrogen donor. CuCs(2)-MCM achieved a 99.6% FFA yield at an optimized reaction conditions of 170 ℃, 1 h. Cu species in CuCs(2)-MCM had dual functions in catalytically decomposing formic acid to generate hydrogen and hydrogenating FF to FFA. The doping of Cs made the size of Cu particles smaller and improved the dispersion of the Cu active sites. Importantly, the Cs species played a favorable role in enhancing the hydrogenation activity as a promoter by adjusting the surface acidity of Cu species to an appropriate level. Correlation analysis showed that surface acidity is the primary factor to affect the catalytic activity of CuCs(2)-MCM.
MoS2 has emerged for catalyzing the hydrogen evolution reaction. Various notable strategies have been developed to downsize the MoS2 particles and expose more active edges. However, the restacking issue, which reduces the exposure degree, has rarely been taken into account. Herein, we report on a facile proton-induced fast hydrothermal approach to produce size-controllable MoS2 nanocatalysts and demonstrate that along the varying of sheet sizes, there is a trade-off between the intrinsic catalytic activity (mainly determined by the unsaturated sulfur on the sheet edges) and the active edge accessibility (influenced by the assembly structure). The size-optimized catalyst delivers a high performance of a low overpotential of ~200 mV at 10 mA/cm2, a Tafel slope of 46.3 mV/dec, and a stable working state, which is comparable to the recent notable works. Our findings will provide a pathway for its large-scale application and enhance the water electrolysis performance.
Radiotherapy is commonly used to treat advanced pancreatic cancers and can improve survival by 2 months in combination with gemcitabine. However, prognosis and survival improvement remain unsatisfactory, and effective therapies are urgently needed. Piperlongumine has been demonstrated to have therapeutic potentials against various cancers. In this study, we synthesized a series of piperlongumine derivatives and provided evidence that piperlongumine derivatives could be used as effective radiosensitizers in pancreatic cancer. Two compounds enhanced the radiosensitivity of Panc-1 and SW1990 cells. In a pancreatic bi-flank xenograft tumor model, they significantly inhibited tumor growth. Piperlongumine derivatives could induce reactive oxygen species (ROS) expression and regulate the Keap1-Nrf2 protective pathway with enhancement of radiation-induced DNA damage, G2/M-phase cell cycle arrest, and apoptosis. Collectively, our data offer a proof of concept for the use of piperlongumine derivatives as a novel class of radiosensitizers for the treatment of pancreatic cancer.
Tsaokols A (1) and B (2), two complicated flavanol-monoterpenoid hybrids, were isolated from the dried fruits of Amomum tsao-ko under the guidance of LCMS and bioassay. Their structures were determined by extensive spectroscopic analyses and electronic circular dichroism (ECD) calculations. Compounds 1 and 2 shared a flavanol backbone fused with 5/7 and 5/6 bicyclic monoterpenoid scaffolds, which were biogenetically condensed by Michael addition and acetalization. Compounds 1 and 2 exhibited significant α-glucosidase inhibitory activity with IC50 values of 18.8 and 38.6 μmol/L (acarbose, IC50 = 213 μmol/L). Docking study supported the strong interactions of 1 and 2 bonding with enzyme by mainly hydrophobic and hydrogen-bond effects. Compounds 1 and 2 could be fast distinguished by the diagnostic ions at m/z 289 and 313 in negative MS2 experiments.
To date, investigations onto the regulation of reactants mass transfer has been paid much less attention in environmental catalysis. Herein, we demonstrated that by rationally designing the adsorption sites of multi-reactants, the pollutant destruction efficiency, product selectivity, reaction stability and secondary pollution have been all affected in the catalytic chlorobenzene oxidation (CBCO). Experimental results revealed that the co-adsorption of chlorobenzene (CB) and gaseous O2 at the oxygen vacancies of CeO2 led to remarkably high CO2 generation, owning to their short mass transfer distance on the catalyst surface, while their separated adsorptions at Brönsted HZSM-5 and CeO2 vacancies resulted in a much lower CO2 generation, and produced significant polychlorinated byproducts in the off-gas. However, this separated adsorption model yielded superior long-term stability for the CeO2/HZSM-5 catalyst, owning to the protection of CeO2 oxygen vacancies from Cl poisoning by the preferential adsorption of CB on the Brönsted acidic sites. This work unveils that design of environmental catalysts needs to consider both of the catalyst intrinsic property and reactant mass transfer; investigations of the latter could pave a new way for the development of highly efficient catalysts towards environmental pollution control.
Developing highly efficient nickel or iron based hydroxide electrocatalysts is primary essential but challenging for oxygen evolution reaction (OER) at ultra-high current densities. Herein, we developed a facile method to prepare nitrogen and iron doped nickel(Ⅱ) hydroxide nanosheets on self-supported conductive nickel foam (denoted as Fe, N-Ni(OH)2/NF) through ammonia hydrothermal and impregnation methods. Owing to the optimization of the electronic structure by nitrogen doping and the strong synergistic effect between Fe and Ni(OH)2, the three-dimensional (3D) Fe, N-Ni(OH)2/NF nanosheets delivered superior electrocatalytic OER performances in basic solution with low potentials of 1.57V and 1.59V under 500mA/cm2 and 1000mA/cm2 respectively and robust operation for 10 h with ignored activity decay, comparing well with the potentials of previously reported NiFe based electrocatalysts as well as the benchmark commercial Ir/C/NF. In-situ Raman spectroscopy revealed that the main active species were NiOOH during the OER process. The present results are expected to provide new insights into the study of OER process towards ultra-high current densities.
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