Synthesis of mordenite by solvent-free method and its application in the dimethyl ether carbonylation reaction

Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.

Solvent-free fabrication of broadband WS2 photodetectors on paper

Paper-based devices have attracted extensive attention due to the growing demand for disposable flexible electronics.Herein,we integrate semiconducting devices on cellulose paper substrate through a simple abrasion technique that yields high-performance photodetectors.A solvent-free WS_(2) film deposited on paper favors an effective electron-hole separation and hampers recombination.The as-prepared paper-based WS2 photodetectors exhibit a sensitive photoresponse over a wide spectral range spanning from ultraviolet(365 nm)to near-infrared(940 nm).Their responsivity value reaches up to~270 mA W^(−1) at 35 V under a power density of 35 mW cm^(−2).A high performance photodetector was achieved by controlling the environmental exposure as the ambient oxygen molecules were found to decrease the photoresponse and stability of the WS_(2) photodetector.Furthermore,we have built a spectrometer using such a paperbased WS_(2) device as the photodetecting component to illustrate its potential application.The present work could promote the development of cost-effective disposable photodetection devices.

Extraction of Cinnamomum longepaniculatum deciduous leaves essential oil using solvent-free microwave extraction: Process optimization and quality evaluation

The optimal process conditions for solvent-free microwave extraction(SFME)of essential oils from Cinnamomum longepaniculatum deciduous leaves after moisture conditioning were established by response surface methodology(RSM).A Box-Behnken design(BBD)was applied to evaluate the effects of three independent variables:moisture content(A:54%–74%),microwave power(B:300–500 W)and microwave time(C:20–40 min),on the extraction yield of essential oil.The compounds of the essential oils obtained by SFME,hydro-distillation and microwaveassisted hydro-distillation(MADE)were identified by gas chromatography-mass spectrometry(GC-MS),and the total lipids of C.longepaniculatum fresh leaves and deciduous leaves were analyzed.The correlation analysis of the response regression model indicated that quadratic polynomial model could be employed to optimize the extraction of essential oil.The optimal extraction condition was A:58%,B:400 W and C:28 min.In the optimal condition,the maximum extraction yield was 4.475 mL/100 g dw and higher than that by MADE.The main compound of the essential oil was eucalyptol(63.54%),and total oxygenated compounds was 78.95%,mainly caused by SFME and the metabolism of endophytic bacteria with decreasing content of phospholipids and fatty acids.Analysis of variance under the extraction condition illustrated high fitness of the model and the success of RSM for optimizing and reflecting the expected process condition.SFME combined with moisture regulation was an effective method for extracting essential oil from C.longepaniculatum deciduous leaves.

Highly efficient synthesis of β-amino esters via Mannich-type reaction under solvent-free conditions using ZnCl_2 catalyst

β-Amino esters were synthesized via ZnCl2-catalyzed Mannich-type reaction of imines and malonate esters under solvent-free conditions in 6 min. The β-amino ester was converted into the corresponding aspartic acid derivatives.

Solvent-Free Synthesis of Ultrafine Tungsten Carbide Nanoparticles-Decorated Carbon Nanosheets for Microwave Absorption

Carbides/carbon composites are emerging as a new kind of binary dielectric systems with good microwave absorption performance.Herein,we obtain a series of tungsten carbide/carbon composites through a simple solvent-free strategy,where the solid mixture of dicyandiamide(DCA)and ammonium metatungstate(AM)is employed as the precursor.Ultrafine cubic WC1-x nanoparticles(3-4 nm)are in situ generated and uniformly dispersed on carbon nanosheets.This configuration overcomes some disadvantages of conventional carbides/carbon composites and is greatly helpful for electromagnetic dissipation.It is found that the weight ratio of DCA to AM can regulate chemical composition of these composites,while less impact on the average size of WC1-x nanoparticles.With the increase in carbon nanosheets,the relative complex permittivity and dielectric loss ability are constantly enhanced through conductive loss and polarization relaxation.The different dielectric properties endow these composites with distinguishable attenuation ability and impedance matching.When DCA/AM weight ratio is 6.0,the optimized composite can produce good microwave absorption performance,whose strongest reflection loss intensity reaches up to-55.6 dB at 17.5 GHz and qualified absorption bandwidth covers 3.6-18.0 GHz by manipulating the thickness from 1.0 to 5.0 mm.Such a performance is superior to many conventional carbides/carbon composites.

Efficient synthesis of bis(indolyl) methanes catalyzed by(PhCH_2PPh_3)^+Br_3^- under solvent-free conditions

Benzyltriphenylphosphonium tribromide（BTPTB） has been applied as an efficient catalyst for the preparation of bis（indolyl）-methanes （BIMs） via electrophilic substitution of indoles with aldehydes in the absence of solvent.

Bio-Based Hyperbranched Toughener From Tannic Acid and Its Enhanced Solvent-Free Epoxy Resin with High Performance

It is essential to design economic and efficient tougheners to prepare high-performance epoxy resin;however,this has remained a huge challenge.Herein,an eco-friendly,low-cost,and facile-fabricated bio-based hyperbranched toughener,carboxylic acid-functionalized tannic acid(CATA),was successfully prepared and applicated to the preparation of solvent-free epoxy resins.The mechanical performance,morphology,structural characterization,and thermal characterization of toughened epoxy resin system were studied.The toughened epoxy resin system with only 1.0wt%CATA reached the highest impact strength,111%higher than the neat epoxy resin system.Notably,the tensile strength and elongation at break of toughened epoxy resin systems increased moderately with increasing CATA loading.Nonphase-separated hybrids with significant toughening effect were obtained.Additionally,the thermal stabilities of toughened epoxy resin systems decreased with increasing CATA loading.This study provides an eco-friendly,cost-effective,and facile approach for the preparation of high-performance,solvent-free epoxy resins with potential for practical applications in sealing integrated circuits and electrical devices fields.

A convenient synthesis of pyrroles catalyzed by acidic resin under solvent-free condition

A convenient and effective Paal-Knorr condensations of 2,5-hexanedione with most amines have been carried out at room temperature under solvent-free condition.Macroporous strongly acidic styrol resin(D001) as a novel,efficient,cost-effective,and reusable solid acid catalyst for the synthesis of pyrroles under the same conditions.The pyrroles were obtained in high yields in short reaction times.

An efficient and solvent-free one-pot synthesis of dihydropyrimidinones under microwave irradiation

An efficient synthesis of 3,4-dihydropyrimidin-2(1H)-one derivatives using formic acid as catalyst, from aldehydes, β-ketoester and urea(thiourea) without solvent under the irradiation of microwave is described. Compared with the classical Biginelli reaction, this new method has the advantage of good yields (77–94% for aromatic aldehydes) and short reaction time (3–8 min).

Silica supported sodium hydrogen sulfate(NaHSO_4/SiO_2):A mild and efficient reusable catalyst for the synthesis of aryl-14-H-dibenzo[a,j]xanthenes under solvent-free conditions

A simple and efficient procedure for the preparation of aryl- 14-H-dibenzo [aj]xanthenes by a one-pot condensation reaction of 2-naphthol and aryl aldehydes, in the presence of silica supported sodium hydrogen sulfate （NaHSO4/SiO2） as a catalyst and in the absence of solvent has been developed. The present method offers several advantages such as excellent yields, short reaction time （10-30min）, mild condition, simple work-up, and the use of a cheap and environmentally friendly catalyst with remarkable reusability.

V(HSO_4)_3 catalyzed chemoselectivity acetylation of alcohols and phenols in solution and under solvent-free conditions

A variety of alcohols and phenols are efficiently acetylated with acetic anhydride in the presence of a catalytic amount of V（HSO4）3 in solution and under solvent free conditions. Mild reaction conditions, high yields of the products, easy procedure and selective acetylation of alcohols and phenols in the presence of amines and thiols are the main advantages of this procedure.

BF_3·OEt_2 Promoted Solvent-free Synthesis of Benzimidazole Derivatives

Differently substituted benzimidazoles have been synthesized in very good yields in solvent-free conditions from o-phenylenediamine and aldehydes in the presence of BF3·OEt2 as a catalyst. The method is applicable to aromatic, unsaturated and aliphatic aldehydes and to substituted o-phenylenediamines without significant differences.

Solvent-free Synthesis of Dihydrofuran-fused [60]Fullerene Derivatives by High-speed Vibration Milling

Solvent-free reactions of 1, 3-cyclohexanedione, 5, 5-dimethyl-1, 3-cyclohexanedione, 2, 4-pentanedione and ethyl acetoacetate with C60 in the presence of Mn（OAc）3·2H2O and ceric ammonium nitrate （CAN） under the high-speed vibration milling conditions afforded dihydrofuran-fused C60 derivatives. CAN is the better oxidant than Mn（OAc）3·2H2O in these mechanochemical reactions.

One-pot synthesis of tri- and tetra-substituted imidazoles using sodium dihydrogen phosphate under solvent-free conditions

Sodium dihydrogen phosphate （NaH2PO4） efficiently catalyzes the condensation reaction of benzil, aldehydes, amines and ammonium acetate in a four-component reaction under solvent-free conditions. The reaction proceeds rapidly and affords the corresponding tetra-substituted imidazoles in high yields. Also an efficient route was developed for the synthesis of tri-substituted imidazoles from condensation of benzil, aldehydes and ammonium acetate using NaH2PO4.

Strontium chloride-catalyzed one-pot synthesis of 4(3H)-quinazolinones under solvent-free conditions

Strontium chloride was used as an efficient and recyclable catalyst in one-pot condensation of anthranilic acid, ortho esters and amines leading to the formation of 4（3H）-quinazolinone derivatives in good yields at room temperature under solvent-free conditions.

Controlling the Properties of Solvent-free Fe_3O_4 Nanofluids by Corona Structure

We studied the relationship between corona structure and properties of solvent-free Fe3O4 nanofluids. We proposed a series of corona structures with different branched chains and synthesize different solvent-free nanofluids in order to show the effect of corona structure on the phase behavior, dispersion, as well as rheology properties. Results demonstrate novel liquid-like behaviors without solvent at room temperature. Fe3O4 magnetic nanoparticles content is bigger than 8% and its size is about 23 nm. For the solvent-free nanofluids,the long chain corona has the internal plasticization, which can decrease the loss modulus of system, while the short chain of corona results in the high viscosity of nanofluids. Long alkyl chains of modifiers lead to lower viscosity and better flowability of nanofluids. The rheology and viscosity of the nanofluids are correlated to the microscopic structure of the corona, which provide an in-depth insight into the preparing nanofluids with promising applications based on their tunable and controllable physical properties.

Silica triflate as an efficient reagent for the solvent-free synthesis of coumarins

Silica triflate, as a new silica-based reagent, can be used for the efficient synthesis of 4-substituted coumarins via a Pechmann reaction under solvent-free reaction conditions. All reactions were performed at 80 ℃ in good to high yields.

Reductive amination of aldehydes and ketones using sodium borohydride in the presence of silica chloride under solvent-free conditions

A simple and convenient procedure for the preparation of amines from aldehydes and ketones with sodium borohydride activated by silica chloride as a catalyst under solvent-free conditions is described.A variety of aliphatic and aromatic aldehydes,ketones and amines when mixed with NaBH;/silica chloride at room temperature,afforded excellent yield of the corresponding amines.

Efficient one-pot synthesis of 14-substituted-14H-dibenzo[a,j]xanthenes using boric acid under solvent-free conditions

Boric acid efficiently catalysed the one-pot reaction of alkyl or aryl aldehydes with 2-naphthol to afford the corresponding 14- alkyl-or aryl-14H-dibenzo[a,j]xanthenes in good yields under solvent-free conditions.