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A computational study of the catalytic aerobic epoxidation of propylene over the coordinatively unsaturated metal-organic framework Fe(btc): formation of propylene oxide and competing reactions.

The aerobic epoxidation of propylene over the metal-organic framework Fe(btc)(btc = 1,3,5-benzentricarboxylate) as catalyst has been investigated by means of density functional calculations. The mechanisms of the reaction towards propylene oxide, carbonylic products (acetone and propanal) and a pi-allyl radical were investigated to assess the efficiency of Fe(btc)for the selective formation of propylene oxide. Propylene oxide and carbonylic products are formed on Fe(btc)by proceeding via propyleneoxy intermediates in the first step. Subsequently, the intermediates can then either be transformed to propylene oxide by way of ring closure of the intermediate or to the carbonylic compounds of propanal and acetone via 1,2-hydride shift. The results show that the formation of propylene oxide is favored over the formation of carbonylic products mainly due to the activation barriers being 2-3 times smaller. The activation barriers for the formation of the propyleneoxy intermediates on the Fe(btc)catalyst for the first and second reaction cycle are also lower than the barriers obtained for the formation of the pi-allyl radical that acts as the precursor to combustion products. On the basis of these computational results, we therefore expect a high catalytic selectivity of the Fe(btc)catalyst with respect to the formation of propylene oxide. We also compared the catalytic activities of Fe(btc)and Cu(btc). The activation energy of the rate-determining step is almost 2 times lower for Fe(btc)than that for Cu(btc), due to a larger charge transfer from the catalytic site to the Omolecule in the case of Fe(btc).

2539 related Products with: A computational study of the catalytic aerobic epoxidation of propylene over the coordinatively unsaturated metal-organic framework Fe(btc): formation of propylene oxide and competing reactions.

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Minocycline through attenuation of oxidative stress and inflammatory response reduces the neuropathic pain in a rat model of chronic constriction injury.

Several lines of evidence showed that minocycline possesses antioxidant and anti-inflammatory properties. This study aimed to demonstrate the effects of minocycline in rats subjected to chronic constriction injury (CCI).

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Toxicological effect of underutilized plant, Cleistanthus collinus leaf extracts against two major stored grain pests, the rice weevil, Sitophilus oryzae and red flour beetle, Tribolium castaneum.

Toxicity and repellency activity of Cleistanthus collinus (Roxb.) (CC) leaf extracts were evaluated against rice weevil, Sitophilus oryzae (L.) and red flour beetle, Tribolium castaneum (Herbst) under laboratory condition. Five concentration(s) (1%, 1.5%, 2%, 2.5% and 4%) with two controls (acetone and water) treatments along with deltamethrin were used for direct and contact residual toxicity. The insect that survived after CC exposure were transferred to an untreated feeding substrate and the population buildup of subsequent two generation were recorded after 30 (F) and 60 days (F). In the contact residual toxicity, highest CC concentration (4%) produced 75% mortality in S. oryzae and 62.5% mortality in T. castaneum during 7 days of exposure, whereas in direct toxicity the mortality were 81% and 58% respectively, for S. oryzae and T. castaneum. The long term effect of CC was apparent in both the insect species, where Fpopulations were significantly decreased in the CC treatments. CC treatment at 4% produced similar adult mortality in comparison to deltamethrin at 1%. In addition, repellent activity of CC extracts was observed against both S. oryzae and T. castaneum. This is the first step towards assessing the scientific basis for the understanding the effectiveness of CC extracts against stored grain pests and it could be a viable eco-friendly option for stored grain insect pest management.

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Resistance to deltamethrin by domestic and wild Triatoma infestans populations in the municipality of Toro Toro, Potosi, Bolivia.

Chemical control with pyrethroid insecticides has been effective in reducing endemic areas of distribution of Triatoma infestans in the Southern Cone, as well as Bolivia; this had considerably reduced the infestation of households in a large part of the territory. Nowadays, areas such as the Chaco and the Inter-Andean Valleys are regions where the reach of vector control strategies is becoming limited, and infestations of insecticide-treated households are reported more often. The objective of this study was to determine if the persistence of T. infestans stems from changes in the susceptibility of its toxicological profile in four communities in the municipality of Toro Toro, Potosi, Bolivia.

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Influence of chloride on the 185 nm advanced oxidation process.

The use of 185 nm radiation from a conventional low pressure mercury lamp generates the hydroxyl radical (OH) from the photolysis of water and offers an advanced oxidation process (AOP) for water treatment that does not require chemical addition. However, the influence of the water matrix on the process differs substantially from that of other ultraviolet and ozone based processes. In particular chloride (Cl), and not water, absorbs the majority of 185 nm photons when [Cl]>20mgLand generates the chlorine atom radical (Cl) as a reactive species. Evidence suggests that when Clis present, Cl and OH both contribute to contaminant degradation to varying extents. Using nonselective (carbamazepine) and selective (nitrobenzene) radical probes, as well as nonselective (t-butanol), and selective (acetone and acetate) radical scavengers, the influence of Cl, and therefore 185 nm AOP treatment efficiency, is observed to strongly depend on four independent second-order radical rate constants. Furthermore, ionic strength effects support the assumption that Cl is in equilibrium with the relatively nonreactive dichlorine radical anion ().

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Evanescent field refractometry in planar optical fiber.

This Letter demonstrates a refractometer in integrated optical fiber, a new optical platform that planarizes fiber using flame hydrolysis deposition (FHD). The unique advantage of the technology is survivability in harsh environments. The platform is mechanically robust, and can survive elevated temperatures approaching 1000°C and exposure to common solvents, including acetone, gasoline, and methanol. For the demonstrated refractometer, fabrication was achieved through wet etching an SMF-28 fiber to a diameter of 8 μm before FHD planarization. An external refractive index was monitored using fiber Bragg gratings (FBGs), written into the core of the planarized fiber. A direct comparison to alternative FBG refractometers is made, for which the developed platform is shown to have comparable sensitivity, with the added advantage of survivability in harsh environments.

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Cosolvent Effects on Polymer Hydration Drive Hydrophobic Collapse.

Water-mediated hydrophobic interactions play an important role in self-assembly processes, aqueous polymer solubility, and protein folding, to name a few. Cosolvents affect these interactions however the implications for hydrophobic polymer collapse and protein folding equilibria are not well-understood. This study examines cosolvent effects on the hydrophobic collapse equilibrium of a generic 32-mer hydrophobic polymer in urea, trimethylamine-N-oxide (TMAO), and acetone aqueous solutions using molecular dynamics simulations. Our results unveil a remarkable cosolvent concentration-dependent behavior. Urea, TMAO, and acetone all shift the equilibrium towards collapsed structures below 2 M cosolvent concentration and, in turn, to unfolded structures at higher cosolvent concentrations, irrespective of the differences in cosolvent chemistry and the nature of cosolvent-water interactions. We find that weakly attractive polymer-water van der Waals interactions oppose polymer collapse in pure water, corroborating related observations reviewed by Ben-Amotz (Ann. Rev. Phys. Chem. 2016, 67, 617-638). The cosolvents studied in the present work, adsorb at the polymer/water interface and expel water molecules into the bulk, thereby effectively removing the dehydration energy penalty that opposes polymer collapse in pure water. At low cosolvent concentrations, this leads to cosolvent-induced stabilization of collapsed polymer structures. Only at sufficiently high cosolvent concentrations, polymer-cosolvent interactions favor polymer unfolding.

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Highly Selective and Rapid Breath Isoprene Sensing Enabled by Activated Alumina Filter.

Isoprene is a versatile breath marker for non-invasive monitoring of high blood cholesterol levels as well as for influenza, end-stage renal disease, muscle activity, lung cancer and liver disease with advanced fibrosis. Its selective detection in complex human breath by portable devices (e.g. metal-oxide gas sensors), however, is still challenging. Here, we present a new filter concept based on activated alumina powder enabling fast and highly selective detection of isoprene at the ppb level and high humidity. The filter contains high surface area adsorbents that retain hydrophilic compounds (e.g. ketones, alcohols, ammonia) representing major interferants in breath while hydrophobic isoprene is not affected. As a proof-of-concept, filters of commercial activated alumina powder are combined with highly sensitive but rather non-specific, nanostructured Pt-doped SnOsensors. This results in fast (10 s) measurement of isoprene down to 5 ppb at 90% relative humidity with outstanding selectivity (>100) to breath-relevant acetone, ammonia, ethanol and methanol, superior to state-of-the-art isoprene sensors. Most importantly, when exposed continuously to simulated breath mixtures (four analytes) for eight days, this filter-sensor system showed stable performance. It can be incorporated readily into a portable breath isoprene analyzer promising for simple-in-use blood cholesterol monitoring or other patho/physiological conditions.

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Insights into Pore Size Control in Cellulose Nanopapers Through Modeling and Experiments.

An easy way of controlling pore sizes during the preparation of cellulose nanopapers using nanofibrillated cellulose and different solvents, such as water, ethanol and acetone, was applied in this study. A possible mathematical model is also presented, that describes the occuring processes, which model is based on simple probability theory computations taking the number of possible hydrogen bonds into consideration. This model allows the better understanding of the solvent dependence of pore formation on a molecular level. For the comparison of the effects of solvents two different series of cellulose nanopapers were prepared. In the cases of both series, an aqueous nanofibrillated cellulose suspension was used for the fabrication of nanopapers, and different solvents were used for their modification. Based on scanning electron microscopy images and mercury intrusion porosimetry data it has been concluded, that using different solvents was a crucial point in controlling pore sizes. A theory about the swelling effects, as well as the formation and decomposition of nanofibrillated cellulose aggregates based on the hydrogen bonding abilities of the solvents, was proposed and proven in this paper. As-prepared nanocellulose papers can be excellent candidates for further applications as support materials (e.g., virus filtration).

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L-Cysteine Capped CdSe Quantum Dots Synthesized by Photochemical Route.

L-cysteine capped CdSe quantum dots were synthesized via photochemical route in aqueous solution under UV photo-irradiation. The as grown CdSe quantum dots exhibit broad fluorescence at room temperature. The CdSe quantum dots were found to be formed only through the reactions of the precursors, i.e., Cd(NH3)2+4 and SeSO2-3 with the photochemically generated 1-hydroxy-2-propyl radicals, (CH3)2COH radicals, which are formed through the process of H atom abstraction by the photoexcited acetone from 2-propanol. L-Cysteine was found to act as a suitable capping agent for the CdSe quantum dots and increases their biocompatability. Cytotoxicty effects of these quantum dots were evaluated in Chinese Hamster Ovary (CHO) epithelial cells, indicated a significant lower level for the L-cysteine capped CdSe quantum dots as compare to the bare ones.

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