Ammonium chloride-catalyzed green multicomponent synthesis of dihydropyrazine and tetrahydrodiazepine derivatives “on water”

Molecular Diversity - This research describes a simple and efficient one-pot synthetic approach for the preparation of tetrahydrodiazepine and dihydropyrazine (or dihydroquinoxaline) derivatives in...     

VCl3 catalyzed imine-based multicomponent reactions for the facile access of functionalized tetrahydropyridines and β-amino carbonyls

Abstract  

A simple, mild, and highly efficient method has been developed for the preparation of functionalized tetrahydropyridines and β-amino carbonyls from the multicomponent reactions involving in situ imines and vanadium (III) chloride as a Lewis acid. The multicomponent reaction of two equivalents of aromatic aldehyde, two equivalents of amine, and one equivalent β-keto ester in the presence of catalytic amount of VCl₃ provides highly atom economic five-component tetrahydropyridines in very good yields. The same catalyst was found useful for the efficient synthesis of a wide variety of β-amino ketones using direct-type Mannich reaction of aromatic aldehyde, amine, and aromatic ketones. The notable advantages of this method are simple procedure, short reaction time and good yields, and applicable to broad range of substrates.     

Ultrasonically assisted hydrothermal synthesis of activated carbon–HKUST-1-MOF hybrid for efficient simultaneous ultrasound-assisted removal of ternary organic dyes and antibacterial investigation: Taguchi optimization

Activated carbon (AC) composite with HKUST-1 metal organic framework (AC–HKUST-1 MOF) was prepared by ultrasonically assisted hydrothermal method and characterized by FTIR, SEM and XRD analysis and laterally was applied for the simultaneous ultrasound-assisted removal of crystal violet (CV), disulfine blue (DSB) and quinoline yellow (QY) dyes in their ternary solution. In addition, this material, was screened in vitro for their antibacterial actively against Methicillin-resistant Staphylococcus aureus (MRSA) and Pseudomonas aeruginosa (PAO1) bacteria. In dyes removal process, the effects of important variables such as initial concentration of dyes, adsorbent mass, pH and sonication time on adsorption process optimized by Taguchi approach. Optimum values of 4, 0.02 g, 4 min, 10 mg L⁻¹ were obtained for pH, AC–HKUST-1 MOF mass, sonication time and the concentration of each dye, respectively. At the optimized condition, the removal percentages of CV, DSB and QY were found to be 99.76%, 91.10%, and 90.75%, respectively, with desirability of 0.989. Kinetics of adsorption processes follow pseudo-second-order model. The Langmuir model as best method with high applicability for representation of experimental data, while maximum mono layer adsorption capacity for CV, DSB and QY on AC–HKUST-1 estimated to be 133.33, 129.87 and 65.37 mg g⁻¹ which significantly were higher than HKUST-1 as sole material with Q_m to equate 59.45, 57.14 and 38.80 mg g⁻¹, respectively.     

Rapid and efficient synthesis of colloidal gold nanoparticles by?arc discharge method

The microstructural (XRD and SEM) and dielectric behavior of Pb(Zr_0.54Ti_0.46)O₃ (PZT 54/46) ceramic system with donor (La, Nb and La+Nb) doping was studied. For all Nb-doped PZT samples, only one (tetragonal) phase was found, which confirms the compositional shifts near the morphotropic phase boundary. For La- and La+Nb-doped samples, there are two (rhombohedral and tetragonal) phases. Dielectric characteristic behavior (1/ε) for La- and La+Nb-doped PZT was associated with two-phase transitions: Ferro–Ferro at low temperature and Ferro–Para at Curie temperature. For Nb-doped samples, only one phase transition is observed, which indicates the presence of a single ferroelectric phase.     

A synthesis method based on speech production and articulatory model

l introductionUsing articulatory synthesis to produce formant targeted voices can not only succeed theadvantages of a formant synthesizer, viz., the pitch and formant parameters can be axtificiallyspecified or modified flexibly and easily, but also can facilitate high quality with an articulatorysynthesizer. It is a worthy topic in speech techniques.SpeeCh synthesis has been studied deeply and many attentions have been shifted to utilizing prosody in text-to-speech system. However, the ultimat…     

gem-Difunctionalization of α-diazoarylketones with diaryldiselenides and N-halosuccinimides: facile synthesis of α-halo-α-arylseleno ketones

Molecular Diversity - An efficient synthesis of α-halo-α-arylseleno ketones has been developed via gem-difunctionalization of α-diazoarylketones with diaryldiselenides and...     

Reaction intermediates of methanol synthesis and the water–gas-shift reaction on the ZnO(0001) surface

The polar Zn-ZnO(0001) surface is involved in the catalysis of methanol synthesis and the water–gas-shift reaction. We use density functional theory calculations to explore the favorable binding geometries and energies of adsorption of several molecular species relevant to these reactions, namely carbon monoxide (CO), carbon dioxide (CO₂), water (H₂O) and methanol (CH₃OH). We also consider several proposed reaction intermediates, including hydroxymethyl (CH₂OH), methoxyl (CH₃), formaldehyde (CH₂O), methyl (CH₃), methylene (CH₂), formic acid (HCOOH), formate (HCOO), formyl (HCO), hydroxyl (OH), oxygen (O) and hydrogen (H). For each, we identify the preferred binding geometry at a coverage of 1/4 monolayers (ML), and report calculated vibrational frequencies that could aid in the identification of these species in experiment. We further explore the effects on the binding energy when the adsorbate coverage is lowered to 1/9 and 1/16 ML.     

A facile one-pot ultrasound assisted for an efficient synthesis of 1H-spiro[furo[3,4-b]pyridine-4,3′-indoline]-3-carbonitriles

A convenient one-pot protocol was developed for the synthesis of 1H-spiro[furo[3,4-b]pyridine-4,3′-indoline]-3-carbonitrile derivatives. This reaction was carried out through a three component condensation reaction of isatins, malononitrile, and anilinolactones in the presence of a catalytic amount of Et₃N as an inexpensive and available basic catalyst in THF under ultrasound irradiation. The products were obtained in high yields and short reaction times. The main advantage of this synthetic method is that the obtained products in ultrasonic irradiations are different from classical heating.     

Effects of ultrasound-assisted H2O2 on the solubilization and antioxidant activity of yeast β-glucan

Yeast β-glucan (YG) possess an extensive range of biological activities, such as the inhibition of oxidation, but the poor water solubility of macromolecular YG limits its application. In this study, through the combined degradation of ultrasonic waves and H₂O₂, and the optimization of the main process parameters for solubilizing YG by response surface methodology (RSM), a new product of YG_UH was generated. The molecular weight, structural characteristics and degradation kinetics before and after solubilization were evaluated. The results showed that the optimal solubilization conditions were reaction time: 4 h, ultrasonic power: 3 W/mL, H₂O₂ concentration: 24 %. Under these conditions, ultrasound-assisted H₂O₂ increased the solubility (from 13.60 % to 70.00 %) and reduced molecular weight (from 6.73 × 10⁶ Da to 1.22 × 10⁶ Da). Fourier transform infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), Congo red (CR), scanning electron microscopy (SEM) revealed that ultrasound-assisted H₂O₂ increased the conformation's flexibility greatly, without changing the main structure of YG. More importantly, solubilization of YG improved free radical scavenging activity with YG_UH exhibiting the highest levels of DPPH and ABTS⁺ free radical scavenging activity. These results revealed that ultrasound-assisted H₂O₂ degradation could be a suitable way to increase the solubility of YG for producing value-added YG.     

A comment on “critique of home and sengupta's derivation of a Bell inequality”

We clarify some aspects of our derivation of a Bell-type inequality, in response to a paper by Elby.The following comments refer to Andrew Elby's discussion note immediately following our present paper.(a) We wish to stress that physical distinction between NC and LC is particularly important in the case of local realist theories violating NC for any single system but satisfying LC for any correlated many-component system. Arguments given by Elby do not rule out a reasonable theory violating NC but obeying LC. Therefore, a physically meaningful possibility exists that while Bell's inequality derived from NC is violated for a single system, the inequality derived from LC is satisfied for correlated and spatially separated (non-interacting) systems. It is precisely this possibility which was explored by HS in deriving Bell's inequality from NC.(b) Since Elby's formulation of locality condition necessarily involves a relativistic constraint at the level of individual measurements, it is pointless to discuss its compatibility with predictions derived from non-relativistic quantum mechanics, which is well known to allow superluminal communication by mechanisms such as wavepacket travel or spread. Recently this aspect has been discussed in depth by P. Ghose and D. Home,Phys. Rev. A 43, 6382 (1991). It needs to be stressed that our formulation of LC is in line with the separability condition articulated by Einstein in different contexts; see, for example,J. Franklin Inst. 221, 349 (1936), reprinted inIdeas and Opinions (Crown, New York, 1954), pp. 290–323.On leave from: Department of Physics, Bose Institute, Calcutta 700009, India.     

Ultrasound promoted efficient and green synthesis of β-amino carbonyl compounds in aqueous hydrotropic medium

Ultrasound promoted synthesis of β-amino carbonyl compounds in aqueous hydrotropic medium at ambient temperature is reported. The remarkable features of the new procedure are shorter reaction time, excellent yields in aqueous medium, cleaner reaction profile and simple experimental and work-up procedure.     

An efficient ultrasound-promoted synthesis of the Baylis–Hillman adducts catalyzed by imidazole and l-proline

A convenient protocol was developed for the synthesis of the Baylis–Hillman adducts in the presence of weak Lewis base and l-proline at room temperature under ultrasound irradiation. This method provided the products in good to high yields (65–90%) and reasonable reaction times.     

Wells–Dawson heteropolyacid supported on silica: a highly efficient catalyst for synthesis of 2,4,5-trisubstituted and 1,2,4,5-tetrasubstituted imidazoles

Heteropolyacid H₆P₂W₁₈O₆₂·24H₂O (WD) supported on silica (WD/SiO₂) has been used as an effective catalytic system for the synthesis of various 1,2,4,5-tetrasubstituted imidazoles by four-component condensation of benzil, aldehydes, amines and ammonium acetate under solvent-free conditions. This approach can be useful for three-component synthesis of 2,4,5-trisubstituted imidazoles. The same reactions were repeated by using benzoin instead of benzil.     

A green method for the synthesis of pyrrole derivatives using arylglyoxals, 1,3-diketones and enaminoketones in water or water–ethanol mixture as solvent

Molecular Diversity - Three-component reaction between arylglyoxals, 1,3-dicetones and enaminoketones leads to new polyfunctionalized tetraone derivatives which may be easily converted to...     

A convenient and efficient protocol for the synthesis of acylals catalyzed by Brønsted acidic ionic liquids under ultrasonic irradiation

The synthesis of acylals (1,1-diacetates) via the reactions of aldehydes with acetic anhydride was carried out in 85-97% yields at room temperature under ultrasound irradiation catalyzed by the Br?nsted acidic ionic liquid [bmpy]HSO(4). This method provides several advantages, such as solvent-free conditions, operational simplicity, higher yields, and reduced environmental consequences. The ionic liquid was recovered and reused.     

A review on various aspects of organic synthesis using Comins’ reagent

Molecular Diversity - Recently, researchers have shown great interest in compounds such as triflate and enotriflate that are synthesized by Comins reagent. For the above-mentioned reason, we...     

Ecofriendly laccase–hydrogen peroxide/ultrasound-assisted bleaching of linen fabrics and its influence on dyeing efficiency

This study evaluates the bleaching efficiency of enzymatically scoured linen fabrics using a combined laccase–hydrogen peroxide bleaching process with and without ultrasonic energy, with the goal of obtaining fabrics with high whiteness levels, well preserved tensile strength and higher dye uptake. The effect of the laccase enzyme and the combined laccase–hydrogen peroxide bleaching process with and without ultrasound has been investigated with regard to whiteness value, tensile strength, dyeing efficiency and dyeing kinetics using both reactive and cationic dyes. The bleached linen fabrics were characterized using X-ray diffraction and by measuring tensile strength and lightness. The dyeing efficiency and kinetics were characterized by measuring dye uptake and colour fastness. The results indicated that ultrasound was an effective technique in the combined laccase–hydrogen peroxide bleaching process of linen fabrics. The whiteness values expressed as lightness of linen fabrics is enhanced by using ultrasonic energy. The measured colour strength values were found to be slightly better for combined laccase–hydrogen peroxide/ultrasound-assisted bleached fabrics than for combined laccase–hydrogen peroxide for both reactive and cationic dyes. The fastness properties of the fabrics dyed with reactive dye were better than those obtained when using cationic dye. The time/dye uptake isotherms were also enhanced when using combined laccase–hydrogen peroxide/ultrasound-assisted bleached fabric, which confirms the efficiency of ultrasound in the combined oxidative bleaching process. The dyeing rate constant, half-time of dyeing and dyeing efficiency have been calculated and discussed.     

A facile and flexible process of β-cyclodextrin grafted on Fe3O4 magnetic nanoparticles and host-guest inclusion studies

In this study, a kind of novel surface-functionalized magnetic nanoparticles was fabricated by the Fe₃O₄ nanoparticles surface modification with mono-6-deoxy-6-(p-tolylsulfonyl)-cyclodextrin (6-TsO-β-CD), which were employed to interact with uric acid and their behavior was investigated by electrochemical methods. The architecture has been characterized by powder X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR), transmission electron microscopy (TEM), and thermogravimetric analysis (TGA), which confirmed that cyclodextrins have been effectively functionalized on the surface of Fe₃O₄ nanoparticles. The analyses of vibration sample magnetometer (VSM) verified that the nanoparticles owned good magnetic property. The grafted β-cyclodextrin on the Fe3O4 nanoparticles contributed to as a modified electrode for detecting uric acid with cyclic voltammograms. Electrochemical results revealed that the new materials could exhibit excellent molecules recognition ability and show high electrochemical response. The new nanoparticles simultaneously had unique properties of magnetic nanoparticles and cyclodextrins through combining their individual distinct advantages.     

Preparation of allicin-whey protein isolate conjugates: Allicin extraction by water,conjugates’ ultrasound-assisted binding and its stability,solubility and emulsibility analysis

The instability of allicin makes it easily decomposed into various organic sulfur compounds, resulting in significant decrease in biological activity. In this study, allicin was firstly extracted with water, then bound with whey protein isolates (WPI) which were pretreated by ultrasound to form conjugates, and the stability, water solubility and emulsibility of conjugates were as well investigated. The research results showed that there were no significant differences in the extraction yields of allicin from water, 40% and 80% ethanol. Appropriate frequency (20/40 kHz), power (50 W/L) and time (20 min) of ultrasonic pretreatments significantly increased (P < 0.05) the sulfhydryl groups content of WPI by 35.05% over control, causing improvement in binding ability of protein to allicin. The binding process of allicin-WPI displayed good fit with Elovich kinetic model (R² = 0.9781). The mass retention rate of the conjugates (in 60% combination rate) with ultrasonic pretreating kept at 95.97% after 14 days of storage at 25 °C, whereas allicin’s mass retention rate was only 61.79% at same storage condition. The water solubility of the prepared conjugates was significantly higher than allicin. And with optimal condition ultrasonic pretreatment of WPI, the conjugates showed the highest emulsifying capacity and emulsion stability (49.56 m²/g, 10.06 min). In conclusion, the ultrasonically pretreated allicin-WPI conjugates exhibited better stability, water solubility and emulsifying properties compared to allicin, this expands the application field of allicin.