Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is r...Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is regarded as a promising process depending on the superior electron transfer and visible light utilization of photocatalyst.Herein,the nonstoichiometry MoO_(3-x)with outstanding photoresponse ability is prepared and modified by imidazole-based ionic liquid[C_(12)mim]Cl to upgrade electronic structure.The interface H-bonding between MoO_(3-x)and[C_(12)mim]Cl regard as electronic transfer channel and the recombination of e^(-)-h^(+)pairs is effectively inhibited with the modification of[C_(12)mim]Cl.Deep desulfurization rate of 96.6%can be reached within 60 min and the MoO_(3-x)/[C_(12)mim]Cl(MoC_(12))photocatalyst demonstrated outstanding cyclic stability within 7 cycles in an extraction coupled photocatalytic oxidation desulfurization(ECPODS)system.The study provides a new perspective on enhancing photocatalytic desulfurization through defect engineering and surface modification.展开更多
Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials ...Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.展开更多
The synthesis of 2, 4, 6-triisopropyl-1, 3, 5-trioxane with high yield and desirable selec- tivity from solvent-free cyclotrimerization of isobutyraldehyde catalyzed by ionic liquids was reported in this work.
In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high c...In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high catalytic activity and reusability with good to excellent yields of the desired products.Hammett method has been used to determine the acidity order of these ionic liquids and the results are consistent with the catalytic activities observed in acetalization reaction.Maximum product yield of 93%was observed on using[PSPy][OTf]as catalyst and it can be reused at least 8 times without obvious activity loss.展开更多
In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the a...In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the acidifies of bi-SOaH-functionalized ILs were stronger than that of traditional single-SOaH-functionalized ILs. Their catalytic activities in the synthesis of N-（3-phenyl）-3- oxo-1-（phenylpropyl）acetamide were investigated and they were consistent with their acidities.展开更多
FeCl3-based ionic liquid [Bmim]Br/FeCl3 with lower viscosity was synthesized and its structure was character-ized with FT-IR spectroscopy. The denitrogenation performance of the ionic liquid was investigated using the...FeCl3-based ionic liquid [Bmim]Br/FeCl3 with lower viscosity was synthesized and its structure was character-ized with FT-IR spectroscopy. The denitrogenation performance of the ionic liquid was investigated using the Fushun shale diesel fraction with high nitrogen content. Experimental results showed that the ionic liquid presented good denitrogenation performance and the basic N and total N removal efficiency can reach 95.29% and 89.77% under conditions covering a tem-perature of 30 ℃, an IL/oil mass ratio of 1:1, an extraction time of 30 min, and a settling time of 2 h. Correspondingly, the basic N and total N contents in shale diesel fraction dropped from the original 5454 μg/g and 9832 μg/g to 257 μg/g and 1006 μg/g, respectively. In addition, the basic-N removal efficiency can still reach 60% at an IL/oil mass ratio of 1:7 during four recycles of the ionic liquid.展开更多
A highly selective synthesis of 2,6-dimethylnaphthanlene（2,6-DMN） by transalkylation between 2-methylnaphthanlene（2-MN） and 1,2,4,5-tetramethylbenzene（TeMB） was performed with 1-alkyl-3-methylimidazo- lium alumi...A highly selective synthesis of 2,6-dimethylnaphthanlene（2,6-DMN） by transalkylation between 2-methylnaphthanlene（2-MN） and 1,2,4,5-tetramethylbenzene（TeMB） was performed with 1-alkyl-3-methylimidazo- lium aluminum chloride（[Cnmim]Cl-AlCl3） ionic liquids（ILs） as catalysts. The influences of the alkyl group as the organic cation, the acidic strength of [C4mim]Cl-AlCl3 ILs as well as the reaction conditions on the catalytic performance were investigated. [C4mim]Cl-AlCl3 ILs[x（AlCl3）=71%] exhibited high activity and selectivity toward 2,6-DMN. The selectivity to 2,6-DMN and the 2,6-DMN/2,7-DMN ratio reached up to 68.2% and 3.7：1, respectively. The UV-Vis spectrum of TeMB treated by different ILs shows that the protonated degree of TeMB dependeds on the acidity strength of ILs, which has a significant impact on the reaction results. The high protonated degree of TeMB is advantageous to enhancing the conversion of transalkylation and the large stereo-hindrance effect of TeMB is favorable to improving the selecivity to 2,6-DMN.展开更多
Several 1-vinyl-3-alkylimidazolium halogens [VRIM]X, which are functional materials with ethylenic bonds, were synthesized using the microwave-assisted synthesis method. Fourier transform infrared spectroscopy and 1H ...Several 1-vinyl-3-alkylimidazolium halogens [VRIM]X, which are functional materials with ethylenic bonds, were synthesized using the microwave-assisted synthesis method. Fourier transform infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy were carded out to analyze the resultant structures. The electrochemical properties and solubility of [VRIM]Br were investigated and discussed in detail. The temperature dependence of pure [VRIM]Br over a wide temperature range of 298.15-323.15 K fitted the Arrhanius equation well. At certain low concentrations, the electrical conductivity of the [VRIM]Br solution significantly increased with increasing solution concentration. The electrical conductivities of the [VRIM]Br observed in water, methanol, and ethanol showed the trend σwater〉 σmethanol 〉σethanol Conductometry showed that the critical miceUe concentrations of the bromines in water, methanol, and ethanol were 6.8-6.9 × 10-6, 1.4-1.5 × 10-5, and 1.9-2.0×10-5 mol.L-1, respectively; these results indicate that [VRIM]Br is an excellent surfactant. The solubility of [VRIM]X in common solvents was determined at 293.15 K, and results indicated that a decrease in solubility could be observed with decreasing dielectric constant of the solvent, elongation of the alkyl chain of the cation, and increasing anion size. Solubility parameters were also determined according to the Hildebrand-Scoff equation.展开更多
An efficient and environmental benign method is reported for the condensation of 3-methyl-1-phenyl-5-pyrazolone with carbonyl compounds in ionic liquids [Bmim]BF4 and [Bmim]PF6 catalyzed by ethylenediammonium diacetate.
The reaction of aromatic aldehydes 1 with 5, 5-dimethyl-1, 3-cyclohexandione 2 was investigated in this paper by using [bmim][BF4] as the reaction medium. It was found that when the reaction was carried out in the pre...The reaction of aromatic aldehydes 1 with 5, 5-dimethyl-1, 3-cyclohexandione 2 was investigated in this paper by using [bmim][BF4] as the reaction medium. It was found that when the reaction was carried out in the presence of catalytic amount of FeCl3·6H2O, xanthenediones 3 was obtained in high yields. On the other hand, when a combination of trimethylchlorosilane (TMSCl) and FeCl3·6H2O was employed as the catalyst, the reaction afforded ring-opening derivatives of xanthenediones 4 with high efficiency.展开更多
Silica-grafted N-propyl-imidazolium hydrogen sulfate ([Sipim]HSO4) is employed as a recyclable heterogeneous ionic liquid catalyst for the synthesis of 3,4-dihydropyrano[c]-chromenes by the reaction of aromatic aldehy...Silica-grafted N-propyl-imidazolium hydrogen sulfate ([Sipim]HSO4) is employed as a recyclable heterogeneous ionic liquid catalyst for the synthesis of 3,4-dihydropyrano[c]-chromenes by the reaction of aromatic aldehydes, malononitrile and 4-hydroxycoumarin at 100°C under solvent-free conditions. Also, heterogeneous ionic liquid catalyst was used for the synthesis of pyrano[2,3-c]-pyrazoles by the reaction of aromatic aldehydes, malononitrile and 3-methyl-l-phenyl-5-pyrazolone at 110°C under solvent-free conditions. The heterogeneous ionic liquid showed much the same efficiency when used in consecutive reaction runs.展开更多
In this paper, the effect of ionic liquids on the CaCO3 crystal growth has been studied for the first time. The obtained CaCO3 crystals were charactered by the X-ray diffraction and scanning electron micrographs. The ...In this paper, the effect of ionic liquids on the CaCO3 crystal growth has been studied for the first time. The obtained CaCO3 crystals were charactered by the X-ray diffraction and scanning electron micrographs. The results showed that the control ability of ionic liquids for CaCO3 crystals growth was dependent on the counter anion very much.展开更多
The main advantages of the use of ionic liquids in enhanced oil recovery are their tunability and stability in harsh environmental conditions. In this work, a comprehensive review of ionic liquids proposed to improve ...The main advantages of the use of ionic liquids in enhanced oil recovery are their tunability and stability in harsh environmental conditions. In this work, a comprehensive review of ionic liquids proposed to improve current chemical oil recovery methods has been presented, focusing on core flooding experiments. With an almost infinite number of possible ionic liquids, the amount of experiments carried out up to now has been very limited. However, results are promising, with additional recovery after secondary flooding of up to 32% of the original oil in place. Most formulations with ionic liquids have been proposed for sandstone reservoirs, the number of studies with carbonate cores being very scarce. The possibilities of a new room temperature surface active ionic liquid, 1-decyl-3-methylimidazolium triflate,for this application were analyzed. It was shown that it is able to drastically reduce the water/oil interfacial tension. An optimized formulation was proposed for carbonate reservoirs. After secondary flooding with brine, an additional recovery of 10.5% of original oil in place was achieved at room conditions. A combination of the proposed method followed by a polymer flooding step with polyacrylamide led to a lesser but still significant recovery, reducing the costs associated to the ionic liquid.展开更多
The low-viscosity FeCl_(3)-based ionic liquids(ILs)prepared from the interaction of anhydrous FeCl_(3) and alkyl imidazolium bromide([1-alkyl-3-methyl-imidazolium]Br,alkyl=ethyl,butyl,hexyl,octyl)are highly effective ...The low-viscosity FeCl_(3)-based ionic liquids(ILs)prepared from the interaction of anhydrous FeCl_(3) and alkyl imidazolium bromide([1-alkyl-3-methyl-imidazolium]Br,alkyl=ethyl,butyl,hexyl,octyl)are highly effective for the denitrogenation of model oil containing quinoline or indole.The results indicate that the chain length of the alkyl group on the imidazolium cation has little influence on the N-extraction efficiency.With the selected IL[Bmim]Br/FeCl_(3),up to 99.1%of N-extraction efficiency from model oil containing quinoline can be attained at an extraction temperature of 30°C with an IL/oil mass ratio of 1/7 and an extraction time of 30 min.The indole extraction efficiency reaches 98.9%at an IL/oil mass ratio of 1:1.Moreover,the quinoline extraction efficiency remains as high as 92.3%after the IL has been recycled four times.展开更多
The methylammonium lead triiodide(CH_(3)NH_(3)PbI_(3))-based perovskite shows a great alluring prospect in areas of solar cells, lasers, photodetectors, and light emitting diodes owing to their excellent optical and e...The methylammonium lead triiodide(CH_(3)NH_(3)PbI_(3))-based perovskite shows a great alluring prospect in areas of solar cells, lasers, photodetectors, and light emitting diodes owing to their excellent optical and electrical advantages. However,it is very sensitive to the surrounding oxygen and moisture, which limits its development seriously. It is urgent to spare no effort to enhance its optical and electrical stability for further application. In this paper, we synthesize the MAPbI_(3) perovskite film on the glass substrate with/without the ionic liquid(IL) of 1-Butyl-3-methylimidazolium tetrafluoroborate(BMIMBF_(4)) by a simple two-step sequential solution method. The additive of BMIMBF_(4)can improve the quality of crystal structure. Moreover, the photo-luminescence(PL) intensity of MAPbI_(3) film with BMIMBF_(4) is much stronger than the pure MAPbI_(3) film after a week in the air, which is almost ten-fold of the pure one. Meanwhile, under the illumination of 405-nm continuous wave(CW) laser, the fluorescent duration of the MAPbI_(3) film with BMIMBF_(4) is approximately 2.75 min, while the pure MAPbI;film is only about 6 s. In fact, ionic liquid of BMIMBF_(4) in the perovskite film plays a role of passivation, which prevents the dissolution of MAPbI_(3) into CH_(3)NH_(3)and PbI_(2) and thus enhances the stability of environment. In addition, the ionic liquid of BMIMBF;possesses high ionic conductivity, which accelerates the electron transport, so it is beneficial for the perovskite film in the areas of solar cells, photodetectors, and lasers. This interesting experiment provides a promising way to develop the perovskite’s further application.展开更多
CeF3 and CeF3：Tb3＋ nanocrystals were successfully synthesized by the ultrasound assisted ionic liquid （IL） method at room temperature. X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission ...CeF3 and CeF3：Tb3＋ nanocrystals were successfully synthesized by the ultrasound assisted ionic liquid （IL） method at room temperature. X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, selected area electron diffraction （SAED）, high-resolution transmission electron micrographs （HRTEM） and photoluminescence （PL） spectra were employed to characterize the nanocrystals. The results of XRD indicated that the obtained samples crystallized well with a hexagonal phase crystal structure. SEM and TEM images demonstrated that the obtained CeF3：Tb3＋ nanocrystals had a discoid shapein the presence of ultrasound and IL, whereas only granular nanoparticles were obtained by magnetic stirring. The possible formation mechanisms of the crystal growth were proposed. The PL spectra of the CeF3：Tb3＋ nanodisks exhibited a strong green emission when excited at 254 nm. Furthermore, the photoluminescence intensity of CeF3：Tb3＋ of the discoid particles was largely improved com-pared with that of the granular nanoparticles.展开更多
Abstract The study on the catalysis of ionic liquids for alkylation of benzene with 1-octadecene to synthesize LAB （linear alkylbenzenes） was performed. The results showed that the most important factor that governe...Abstract The study on the catalysis of ionic liquids for alkylation of benzene with 1-octadecene to synthesize LAB （linear alkylbenzenes） was performed. The results showed that the most important factor that governed the conversion of olefin and selectivity of LAB was reaction temperature. Moreover, the effects of different ionic liquids and molar ratio of benzene to 1-octadecene on the conversion and selectivity were obviously in different degrees. The reaction temperature, molar ratio of benzene to 1-octadecene and the amount of catalyst were lower, compared with the traditional reaction technologies. The experimental results demonstrated that the ionic liquid had higher activity at 30℃, with over 98% selectivity of monoalkylbenzene and 100% conversion of the olefin at the molar ratio 0.08 of FeCl3 in ionic liquid to 1-octadecene and 10 for benzene to 1-octadecene.展开更多
The alkylation of toluene with 1,3-pentadiene to produce pentyltoluene was carded out to obtain 2,6-dimethylnaphalene, which is an important intermediate during the production of 2,6-naphthalene dicarboxylic acid. Bas...The alkylation of toluene with 1,3-pentadiene to produce pentyltoluene was carded out to obtain 2,6-dimethylnaphalene, which is an important intermediate during the production of 2,6-naphthalene dicarboxylic acid. Based on our previous work using anhydrous AlCl3 as catalyst, [bupy]BF4-AlCl3 ionic liquids were employed to catalyze the reaction of 1,3-pentadiene with toluene. The experimental results show that [bupy]BF4-AlCl3 ionic liquids are suitable for the reaction especially when the molar ratio of AlCl3 to [bupy]BF4 is 1.75 ： 1, and the reaction could proceed at the temperature as low as 0℃. It could be as active as pure AlCl3, but much more environmentally friendly.展开更多
Up to now the mechanism of Priedel-Crafts reactions catalyzed by ionic liquidhave not been fully understood, while carbocation mechanism was assumed. It was found that thesource of H^+ and the route of reaction initia...Up to now the mechanism of Priedel-Crafts reactions catalyzed by ionic liquidhave not been fully understood, while carbocation mechanism was assumed. It was found that thesource of H^+ and the route of reaction initiated the alkylation of benzene with ethylene catalyzedby [bmim]Cl/FeCl_3 ionic liquid. The fact that dewatered ionic liquids have catalytic activity forthe alkylation of benzene with ethylene suggests that there exists a new catalytic route. Thedistinctly Bronsted acid properties of 2-H in [bmim]Cl were found through FT-IR and HNMR analysis of[bmim]Cl after titration with water free KOH in alcohol solution. In addition, the chemical shiftsof proton on the [bmim]Cl ring, especially 2-H, are sensitive to the change of FeCl_3 content andshifted downfield when FeCl_3 was added into [bmim]Cl to form ionic liquid. Thus 2-H was easy to bedisengaged from imidazolium ring with formation of H^+ to initiate the reaction. Theisotope-substituted method was employed to prove this mechanism, through the GC-MS analysis ofalkylation products of deuterated benzene with ethylene. The route of alkylation catalyzed by FeCl_3ionic liquid was found to follow the carbocation mechanism, the resource of H^+ was presented andproved using HNMR analysis of ionic liquid to inspect the intensity change of 2-H. It was found thatthe intensity of 2-H reduced 23% after reaction showing that the H^+ arising from alkylationreaction was supplied by 2-H on the imidazole ring.展开更多
Promoted and mediated by an ionic liquid-[bmim][BF4], fused pyrans or arylbis（4-hydroxy-6-methyl-2-oxo-2H-pyran-3- yl）methanes were efficiently and selectively prepared from the reaction of aldehyde and 4-hydroxy-6-...Promoted and mediated by an ionic liquid-[bmim][BF4], fused pyrans or arylbis（4-hydroxy-6-methyl-2-oxo-2H-pyran-3- yl）methanes were efficiently and selectively prepared from the reaction of aldehyde and 4-hydroxy-6-methyl-2-oxo-pyran with or without acetic anhydride. By using these novel procedures, pyrimidine nucleoside-fused pyran and arylbis（pyranon-3-yl）methane hybrids with potential biological activities were constructed.展开更多
基金supports from National Natural Science Foundation of China(Nos.22172066,22378176)supported by State Key Laboratory of Heavy Oil Processing.Supported by Jiangsu Collaborative Innovation Center of TechnologyMaterial of Water Treatment,Suzhou University of Science and Technology.
文摘Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is regarded as a promising process depending on the superior electron transfer and visible light utilization of photocatalyst.Herein,the nonstoichiometry MoO_(3-x)with outstanding photoresponse ability is prepared and modified by imidazole-based ionic liquid[C_(12)mim]Cl to upgrade electronic structure.The interface H-bonding between MoO_(3-x)and[C_(12)mim]Cl regard as electronic transfer channel and the recombination of e^(-)-h^(+)pairs is effectively inhibited with the modification of[C_(12)mim]Cl.Deep desulfurization rate of 96.6%can be reached within 60 min and the MoO_(3-x)/[C_(12)mim]Cl(MoC_(12))photocatalyst demonstrated outstanding cyclic stability within 7 cycles in an extraction coupled photocatalytic oxidation desulfurization(ECPODS)system.The study provides a new perspective on enhancing photocatalytic desulfurization through defect engineering and surface modification.
基金financially supported by the National Key R&D Program of China(Grant No.2022YFE0207300)National Natural Science Foundation of China(Grant Nos.22179142 and 22075314)+1 种基金Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2024ZB051 and 2023ZB836)the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO).
文摘Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.
基金We graleully appreciate the financial support from the National Natural Science Foundation of China(G2000048).
文摘The synthesis of 2, 4, 6-triisopropyl-1, 3, 5-trioxane with high yield and desirable selec- tivity from solvent-free cyclotrimerization of isobutyraldehyde catalyzed by ionic liquids was reported in this work.
基金supported by National 863 High-Tech Research and Development Program of China(No. 2007AA05Z101)
文摘In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high catalytic activity and reusability with good to excellent yields of the desired products.Hammett method has been used to determine the acidity order of these ionic liquids and the results are consistent with the catalytic activities observed in acetalization reaction.Maximum product yield of 93%was observed on using[PSPy][OTf]as catalyst and it can be reused at least 8 times without obvious activity loss.
基金the National Natural Science Foundation ofChina(Nos.21003049,21073064)the Fundamental Research Funds for the Central Universities for financial support
文摘In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the acidifies of bi-SOaH-functionalized ILs were stronger than that of traditional single-SOaH-functionalized ILs. Their catalytic activities in the synthesis of N-（3-phenyl）-3- oxo-1-（phenylpropyl）acetamide were investigated and they were consistent with their acidities.
基金financial support from the Doctoral Funds of Liaoning Provincial Natural Science Foundation (201601323)
文摘FeCl3-based ionic liquid [Bmim]Br/FeCl3 with lower viscosity was synthesized and its structure was character-ized with FT-IR spectroscopy. The denitrogenation performance of the ionic liquid was investigated using the Fushun shale diesel fraction with high nitrogen content. Experimental results showed that the ionic liquid presented good denitrogenation performance and the basic N and total N removal efficiency can reach 95.29% and 89.77% under conditions covering a tem-perature of 30 ℃, an IL/oil mass ratio of 1:1, an extraction time of 30 min, and a settling time of 2 h. Correspondingly, the basic N and total N contents in shale diesel fraction dropped from the original 5454 μg/g and 9832 μg/g to 257 μg/g and 1006 μg/g, respectively. In addition, the basic-N removal efficiency can still reach 60% at an IL/oil mass ratio of 1:7 during four recycles of the ionic liquid.
基金Supported by the National Natural Science Foundation of China(No.21076065)the Natural Science Foundation of Heilongjiang Province of China(No.ZD200820-02)the Science&Technology Research Foundation of Education Bureau of Heilongjiang Province,China(No.11531266)
文摘A highly selective synthesis of 2,6-dimethylnaphthanlene（2,6-DMN） by transalkylation between 2-methylnaphthanlene（2-MN） and 1,2,4,5-tetramethylbenzene（TeMB） was performed with 1-alkyl-3-methylimidazo- lium aluminum chloride（[Cnmim]Cl-AlCl3） ionic liquids（ILs） as catalysts. The influences of the alkyl group as the organic cation, the acidic strength of [C4mim]Cl-AlCl3 ILs as well as the reaction conditions on the catalytic performance were investigated. [C4mim]Cl-AlCl3 ILs[x（AlCl3）=71%] exhibited high activity and selectivity toward 2,6-DMN. The selectivity to 2,6-DMN and the 2,6-DMN/2,7-DMN ratio reached up to 68.2% and 3.7：1, respectively. The UV-Vis spectrum of TeMB treated by different ILs shows that the protonated degree of TeMB dependeds on the acidity strength of ILs, which has a significant impact on the reaction results. The high protonated degree of TeMB is advantageous to enhancing the conversion of transalkylation and the large stereo-hindrance effect of TeMB is favorable to improving the selecivity to 2,6-DMN.
基金Funded by the Special Funds of the National Natural Science Foundation of China(No.21174111)
文摘Several 1-vinyl-3-alkylimidazolium halogens [VRIM]X, which are functional materials with ethylenic bonds, were synthesized using the microwave-assisted synthesis method. Fourier transform infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy were carded out to analyze the resultant structures. The electrochemical properties and solubility of [VRIM]Br were investigated and discussed in detail. The temperature dependence of pure [VRIM]Br over a wide temperature range of 298.15-323.15 K fitted the Arrhanius equation well. At certain low concentrations, the electrical conductivity of the [VRIM]Br solution significantly increased with increasing solution concentration. The electrical conductivities of the [VRIM]Br observed in water, methanol, and ethanol showed the trend σwater〉 σmethanol 〉σethanol Conductometry showed that the critical miceUe concentrations of the bromines in water, methanol, and ethanol were 6.8-6.9 × 10-6, 1.4-1.5 × 10-5, and 1.9-2.0×10-5 mol.L-1, respectively; these results indicate that [VRIM]Br is an excellent surfactant. The solubility of [VRIM]X in common solvents was determined at 293.15 K, and results indicated that a decrease in solubility could be observed with decreasing dielectric constant of the solvent, elongation of the alkyl chain of the cation, and increasing anion size. Solubility parameters were also determined according to the Hildebrand-Scoff equation.
文摘An efficient and environmental benign method is reported for the condensation of 3-methyl-1-phenyl-5-pyrazolone with carbonyl compounds in ionic liquids [Bmim]BF4 and [Bmim]PF6 catalyzed by ethylenediammonium diacetate.
基金This work was financially supported by NNSFC(No.20273019)the Science Foundation of Henan Normal University for Young Scholars(No.0307032).
文摘The reaction of aromatic aldehydes 1 with 5, 5-dimethyl-1, 3-cyclohexandione 2 was investigated in this paper by using [bmim][BF4] as the reaction medium. It was found that when the reaction was carried out in the presence of catalytic amount of FeCl3·6H2O, xanthenediones 3 was obtained in high yields. On the other hand, when a combination of trimethylchlorosilane (TMSCl) and FeCl3·6H2O was employed as the catalyst, the reaction afforded ring-opening derivatives of xanthenediones 4 with high efficiency.
文摘Silica-grafted N-propyl-imidazolium hydrogen sulfate ([Sipim]HSO4) is employed as a recyclable heterogeneous ionic liquid catalyst for the synthesis of 3,4-dihydropyrano[c]-chromenes by the reaction of aromatic aldehydes, malononitrile and 4-hydroxycoumarin at 100°C under solvent-free conditions. Also, heterogeneous ionic liquid catalyst was used for the synthesis of pyrano[2,3-c]-pyrazoles by the reaction of aromatic aldehydes, malononitrile and 3-methyl-l-phenyl-5-pyrazolone at 110°C under solvent-free conditions. The heterogeneous ionic liquid showed much the same efficiency when used in consecutive reaction runs.
文摘In this paper, the effect of ionic liquids on the CaCO3 crystal growth has been studied for the first time. The obtained CaCO3 crystals were charactered by the X-ray diffraction and scanning electron micrographs. The results showed that the control ability of ionic liquids for CaCO3 crystals growth was dependent on the counter anion very much.
基金the Ministry of Science and Innovation and State Research Agency for financial support throughout project PGC2018-097342-B-I00, including European Regional Development Fund。
文摘The main advantages of the use of ionic liquids in enhanced oil recovery are their tunability and stability in harsh environmental conditions. In this work, a comprehensive review of ionic liquids proposed to improve current chemical oil recovery methods has been presented, focusing on core flooding experiments. With an almost infinite number of possible ionic liquids, the amount of experiments carried out up to now has been very limited. However, results are promising, with additional recovery after secondary flooding of up to 32% of the original oil in place. Most formulations with ionic liquids have been proposed for sandstone reservoirs, the number of studies with carbonate cores being very scarce. The possibilities of a new room temperature surface active ionic liquid, 1-decyl-3-methylimidazolium triflate,for this application were analyzed. It was shown that it is able to drastically reduce the water/oil interfacial tension. An optimized formulation was proposed for carbonate reservoirs. After secondary flooding with brine, an additional recovery of 10.5% of original oil in place was achieved at room conditions. A combination of the proposed method followed by a polymer flooding step with polyacrylamide led to a lesser but still significant recovery, reducing the costs associated to the ionic liquid.
基金The authors are grateful for financial support from the Doctoral Research Funds of Liaoning Petrochemical University(2019×JJ-006).
文摘The low-viscosity FeCl_(3)-based ionic liquids(ILs)prepared from the interaction of anhydrous FeCl_(3) and alkyl imidazolium bromide([1-alkyl-3-methyl-imidazolium]Br,alkyl=ethyl,butyl,hexyl,octyl)are highly effective for the denitrogenation of model oil containing quinoline or indole.The results indicate that the chain length of the alkyl group on the imidazolium cation has little influence on the N-extraction efficiency.With the selected IL[Bmim]Br/FeCl_(3),up to 99.1%of N-extraction efficiency from model oil containing quinoline can be attained at an extraction temperature of 30°C with an IL/oil mass ratio of 1/7 and an extraction time of 30 min.The indole extraction efficiency reaches 98.9%at an IL/oil mass ratio of 1:1.Moreover,the quinoline extraction efficiency remains as high as 92.3%after the IL has been recycled four times.
基金Project supported by the National Key Research and Development Program of China (Grant No. 2018YFC2001100)the Natural National Science Foundation of China (Grant No. 61574017)+1 种基金the Fundamental Research Funds for Central Universities, China (Grant No. 2017CX10007)the Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, Guangxi University (Grant No. 2020GXYSOF08)。
文摘The methylammonium lead triiodide(CH_(3)NH_(3)PbI_(3))-based perovskite shows a great alluring prospect in areas of solar cells, lasers, photodetectors, and light emitting diodes owing to their excellent optical and electrical advantages. However,it is very sensitive to the surrounding oxygen and moisture, which limits its development seriously. It is urgent to spare no effort to enhance its optical and electrical stability for further application. In this paper, we synthesize the MAPbI_(3) perovskite film on the glass substrate with/without the ionic liquid(IL) of 1-Butyl-3-methylimidazolium tetrafluoroborate(BMIMBF_(4)) by a simple two-step sequential solution method. The additive of BMIMBF_(4)can improve the quality of crystal structure. Moreover, the photo-luminescence(PL) intensity of MAPbI_(3) film with BMIMBF_(4) is much stronger than the pure MAPbI_(3) film after a week in the air, which is almost ten-fold of the pure one. Meanwhile, under the illumination of 405-nm continuous wave(CW) laser, the fluorescent duration of the MAPbI_(3) film with BMIMBF_(4) is approximately 2.75 min, while the pure MAPbI;film is only about 6 s. In fact, ionic liquid of BMIMBF_(4) in the perovskite film plays a role of passivation, which prevents the dissolution of MAPbI_(3) into CH_(3)NH_(3)and PbI_(2) and thus enhances the stability of environment. In addition, the ionic liquid of BMIMBF;possesses high ionic conductivity, which accelerates the electron transport, so it is beneficial for the perovskite film in the areas of solar cells, photodetectors, and lasers. This interesting experiment provides a promising way to develop the perovskite’s further application.
基金Project supported by National Natural Science Foundation of China(21001017,21171160,21376031)the Lotus Scholars Program of Hunan+1 种基金the Natural Science Foundation of Hunan Province(13JJ3068)Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation(2014CL03,2014CL05)
文摘CeF3 and CeF3：Tb3＋ nanocrystals were successfully synthesized by the ultrasound assisted ionic liquid （IL） method at room temperature. X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, selected area electron diffraction （SAED）, high-resolution transmission electron micrographs （HRTEM） and photoluminescence （PL） spectra were employed to characterize the nanocrystals. The results of XRD indicated that the obtained samples crystallized well with a hexagonal phase crystal structure. SEM and TEM images demonstrated that the obtained CeF3：Tb3＋ nanocrystals had a discoid shapein the presence of ultrasound and IL, whereas only granular nanoparticles were obtained by magnetic stirring. The possible formation mechanisms of the crystal growth were proposed. The PL spectra of the CeF3：Tb3＋ nanodisks exhibited a strong green emission when excited at 254 nm. Furthermore, the photoluminescence intensity of CeF3：Tb3＋ of the discoid particles was largely improved com-pared with that of the granular nanoparticles.
基金Supported by the National Natural Science Foundation of China （No.20276038） and Beijing Natural Science Foundation （No.2052010）.
文摘Abstract The study on the catalysis of ionic liquids for alkylation of benzene with 1-octadecene to synthesize LAB （linear alkylbenzenes） was performed. The results showed that the most important factor that governed the conversion of olefin and selectivity of LAB was reaction temperature. Moreover, the effects of different ionic liquids and molar ratio of benzene to 1-octadecene on the conversion and selectivity were obviously in different degrees. The reaction temperature, molar ratio of benzene to 1-octadecene and the amount of catalyst were lower, compared with the traditional reaction technologies. The experimental results demonstrated that the ionic liquid had higher activity at 30℃, with over 98% selectivity of monoalkylbenzene and 100% conversion of the olefin at the molar ratio 0.08 of FeCl3 in ionic liquid to 1-octadecene and 10 for benzene to 1-octadecene.
文摘The alkylation of toluene with 1,3-pentadiene to produce pentyltoluene was carded out to obtain 2,6-dimethylnaphalene, which is an important intermediate during the production of 2,6-naphthalene dicarboxylic acid. Based on our previous work using anhydrous AlCl3 as catalyst, [bupy]BF4-AlCl3 ionic liquids were employed to catalyze the reaction of 1,3-pentadiene with toluene. The experimental results show that [bupy]BF4-AlCl3 ionic liquids are suitable for the reaction especially when the molar ratio of AlCl3 to [bupy]BF4 is 1.75 ： 1, and the reaction could proceed at the temperature as low as 0℃. It could be as active as pure AlCl3, but much more environmentally friendly.
文摘Up to now the mechanism of Priedel-Crafts reactions catalyzed by ionic liquidhave not been fully understood, while carbocation mechanism was assumed. It was found that thesource of H^+ and the route of reaction initiated the alkylation of benzene with ethylene catalyzedby [bmim]Cl/FeCl_3 ionic liquid. The fact that dewatered ionic liquids have catalytic activity forthe alkylation of benzene with ethylene suggests that there exists a new catalytic route. Thedistinctly Bronsted acid properties of 2-H in [bmim]Cl were found through FT-IR and HNMR analysis of[bmim]Cl after titration with water free KOH in alcohol solution. In addition, the chemical shiftsof proton on the [bmim]Cl ring, especially 2-H, are sensitive to the change of FeCl_3 content andshifted downfield when FeCl_3 was added into [bmim]Cl to form ionic liquid. Thus 2-H was easy to bedisengaged from imidazolium ring with formation of H^+ to initiate the reaction. Theisotope-substituted method was employed to prove this mechanism, through the GC-MS analysis ofalkylation products of deuterated benzene with ethylene. The route of alkylation catalyzed by FeCl_3ionic liquid was found to follow the carbocation mechanism, the resource of H^+ was presented andproved using HNMR analysis of ionic liquid to inspect the intensity change of 2-H. It was found thatthe intensity of 2-H reduced 23% after reaction showing that the H^+ arising from alkylationreaction was supplied by 2-H on the imidazole ring.
基金the National Natural Science Foundation of China(No.20772025)the Program for Science & Technology Innovation Talents in Universities of Henan Province(No.2008HASTIT006)the Natural Science Foundation of Department of Education of Henan Province(No.2008A150013).
文摘Promoted and mediated by an ionic liquid-[bmim][BF4], fused pyrans or arylbis（4-hydroxy-6-methyl-2-oxo-2H-pyran-3- yl）methanes were efficiently and selectively prepared from the reaction of aldehyde and 4-hydroxy-6-methyl-2-oxo-pyran with or without acetic anhydride. By using these novel procedures, pyrimidine nucleoside-fused pyran and arylbis（pyranon-3-yl）methane hybrids with potential biological activities were constructed.
