Due to the large number of ionic liquids(ILs)and their potential environmental risk,assessing the toxicity of ILs by ecotoxicological experiment only is insufficient.Quantitative structure-activity relationship(QSAR)h...Due to the large number of ionic liquids(ILs)and their potential environmental risk,assessing the toxicity of ILs by ecotoxicological experiment only is insufficient.Quantitative structure-activity relationship(QSAR)has been proven to be a quick and effective method to estimate the viscosity,melting points,and even toxicity of ILs.In this work,the LC50 values of 30 imidazolium-based ILs were determined with Caenorhabditis elegans as a model animal.Four suitable molecular descriptors were selected on the basis of genetic function approximation algorithm to construct a QSAR model with an R^2 value of 0.938.The predicted lgLC50 in this work are in agreement with the experimental values,indicating that the model has good stability and predictive ability.Our study provides a valuable model to predict the potential toxicity of ILs with different sub-structures to the environment and human health.展开更多
Most of the onshore and offshore oil and gas reservoirs are facing operational challenges due to high temperature and high salinity, thus requiring advanced techniques for realizing the ex- pected oil recovery with th...Most of the onshore and offshore oil and gas reservoirs are facing operational challenges due to high temperature and high salinity, thus requiring advanced techniques for realizing the ex- pected oil recovery with the use of specially designed chemicals. During oil and gas well development, completion fluids, which are solids-free liquids, are used to complete an oil or gas well. Completion flu- ids consisting of brines are primarily used for oil and gas well stabilization and are corrosive in nature. There is a need to develop additives to be added with completion fluids to address the corrosive nature. The present investigation involved the usage of two imidazolium ionic liquids （ILs） as corrosion inhibi- tors for mild steel in various completion brine （CaCI2, HCOOCs and ZnBr2） fluids. The study was per- formed using various techniques, such as, potentiodynamic polarization, weight loss measurements and exposure studies. All the above techniques showed promising results which indicated that the ILs as corrosion inhibitors used were of the mixed-type following both physisorption and chemisorption over the mild steel surface. Among the two inhibitors studied here, l-octyl-3-methyl imidazolium chlo- ride （[OMIM]^＋[CI]^-） with longer alkyl chain exhibited better inhibition efficiency and much lesser cor- rosion rate than 1-butyl-3-methyl imidazolium chloride （[BMIM]^＋[Ci]^-） with a shorter alkyl chain. The results obtained from various methodologies indicate that ionic liquids can be explored to develop anti-corrosive completion fluids suitable for oil and gas reservoirs.展开更多
The separation of methanol(MeOH)and dimethyl carbonate(DMC)is important but difficult due to the formation of an azeotropic mixture.In this work,isobaric vapor–liquid equilibrium(VLE)data for the ternary systems cont...The separation of methanol(MeOH)and dimethyl carbonate(DMC)is important but difficult due to the formation of an azeotropic mixture.In this work,isobaric vapor–liquid equilibrium(VLE)data for the ternary systems containing different imidazolium–based ionic liquids(ILs),i.e.MeOH+DMC+1-butyl-3-methy-limidazolium bis[(trifluoromethyl)sulfonyl]imide([Bmim][Tf2N]),MeOH+DMC+1-ethyl-3-methyl-imidazolium bis[(trifluoromethyl)sulfonyl]imide([Emim][Tf2N]),and MeOH+DMC+1-ethyl-3-methylimidazolium hexafluorophosphate([Emim][PF6])were measured at 101.3 kPa.The mole fraction of IL was varied from0.05 to 0.20.The experimental data were correlated with the NRTL and Wilson equations,respectively.The results show that imidazolium-based ILs were beneficial to improve the relative volatility of MeOH to DMC,and[Bmim][Tf2 N]showed a much more excellent performance on the activity coefficient of MeOH.The interaction energies of system components were calculated using Gaussian program,and the effects of cation and anion on the separation coefficient of the azeotropic system were discussed.展开更多
Three ionic liquids(ILs),1-ethyl-3-methylimidazolium bromine([EMIM]Br),1-butyl-3-methylimidazolium bromine([BMIM]Br),and 1-hexyl-3-methylimidazolium bromine([HMIM]Br),were used as the solvent for separation of {tert-b...Three ionic liquids(ILs),1-ethyl-3-methylimidazolium bromine([EMIM]Br),1-butyl-3-methylimidazolium bromine([BMIM]Br),and 1-hexyl-3-methylimidazolium bromine([HMIM]Br),were used as the solvent for separation of {tert-butyl alcohol(TBA)+ water} azeotrope.Vapor–liquid equilibrium(VLE)data for {TBA + water + IL}ternary systems were measured at 101.3 k Pa.The results indicate that all the three ILs produce an obvious effect on the VLE behavior of {TBA + water} system and eliminate the azeotropy in the whole concentration range.[EMIM]Br is the best solvent for the separation of {TBA + water} system by extractive distillation among the three ILs.The experimental VLE data for the ternary systems are correlated with the NRTL model equation with good correlations.Explanations are given with activity coefficients of water and TBA,and the experimental VLE-temperature data for {TBA or water + IL} binary systems.展开更多
How to completely remove the water from ionic liquids(ILs)is difficult for researchers because of the hygroscopicity of ILs.In order to study the hygroscopicity of ILs,two kinds of ILs,1-Butyl-3-methylimidazolium hexa...How to completely remove the water from ionic liquids(ILs)is difficult for researchers because of the hygroscopicity of ILs.In order to study the hygroscopicity of ILs,two kinds of ILs,1-Butyl-3-methylimidazolium hexafluorophosphate([Bmim][PF6])and 1-Butyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)([Bmim][NTf_(2)])were investigated by molecular dynamics simulations.Although[Bmim][PF6]and[Bmim][NTf_(2)]are hydrophobic,both of the ILs could absorb water molecules from the vapor.In this work,the process of absorbing water from the vapor phase was studied,and the water molecules could disperse into the IL.Aggregation was observed with increasing the water concentration.Although the absorbed water increases obviously,the amount of free water and small cluster in the ILs does not change significantly and always stays at a certain level.The amount of free water and small cluster in[Bmim][PF6]is more than that in[Bmim][NTf_(2)],which is consistent with their hydrophobicity.In addition,the liquid-vacuum and liquid–liquid interfaces of the ILs were simulated and analyzed in detail.The number density distribution and angle distribution indicated that[Bmim]+cations arrangement regularly at the IL-vacuum interface.The butyl chain point to the vacuum,while the imidazlium ring is close to the IL phase region and perpendicular to the interface.While at the IL-water interface,the cations and anions are disordered.展开更多
The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement rema...The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.展开更多
The interactions of bovine serum albumin (BSA) with two alkylimidazolium-based ionic liquids, 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim]BF4) and 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim]PF6), ...The interactions of bovine serum albumin (BSA) with two alkylimidazolium-based ionic liquids, 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim]BF4) and 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim]PF6), in buffer solutions at pH 7.0 were investigated by isothermal titration calorimetry (ITC) and circular dichroism (CD). CD spectra showed that the two ionic liquids changed the secondary structure of BSA. Data process was based on the supposition that there were several independent types of binding sites on each BSA molecule for the two ligand molecules. The results obtained by using this supposition combined with Langmuir adsorption model showed that there were two types of such binding sites. One was the high affinity binding site, and the other was the low affinity binding site. The binding constants, changes in enthalpy, entropy and Gibbs free energy for the two types of binding were obtained, which showed that the two types of binding were driven by a favorable entropy increase. Furthermore, for either the ionic liquids, the number of the high affinity binding sites is much smaller than that of the low affinity ones. These results were interpreted with the molecular structure of BSA and the different substituent groups on imidazole ring of the two ionic liquid molecules.展开更多
In this work,we proposed a strategy for the hydrolysis of native corn starch after the treatment of corn starch in an ionic liquid aqueous solution,and it is an awfully“green”and simple means to obtain starch with l...In this work,we proposed a strategy for the hydrolysis of native corn starch after the treatment of corn starch in an ionic liquid aqueous solution,and it is an awfully“green”and simple means to obtain starch with low molecular weight and amorphous state.X-ray diffraction results revealed that the natural starch crystalline region was largely disrupted by ionic liquid owing to the broken intermolecular and intramolecular hydrogen bonds.After hydrolysis,the morphology of starch changed from particles of native corn starch into little pieces,and their molecular weight could be effectively regulated during the hydrolysis process,and also the hydrolyzed starch samples exhibited decreased thermal stability with the extension of hydrolysis time.This work would counsel as a powerful tool for the development of native starch in realistic applications.展开更多
Separation of 2-methylfuran(2-MF)and methanol(MeOH)azeotropes is a key challenge in biofuel production because of the efficiency and sustainability issues of conventional methods.In this study,ionic liquids(ILs)were i...Separation of 2-methylfuran(2-MF)and methanol(MeOH)azeotropes is a key challenge in biofuel production because of the efficiency and sustainability issues of conventional methods.In this study,ionic liquids(ILs)were introduced as green solvents for separation of 2-MF/MeOH through liquid–liquid equilibrium(LLE)experiment.Three ILs,namely 1-ethyl-3-methylimidazole dihydrogen phosphate([EMIM][H_(2)PO_(4)]),1-propyl-3-methylimidazole dihydrogen phosphate([PMIM][H_(2)PO_(4)])and 1-butyl-3-methylimidazole dihydrogen phosphate([BMIM][H_(2)PO_(4)]),were screened out from 425 candidates using the conductor-like screening model for real solvents(COSMO-RS).Then,the ternary LLE data of 2-MF(1)+MeOH(2)+ILs(3)were determined at 30℃ and 101.32 kPa.Results confirmed[EMIM][H_(2)PO_(4)]as the best performer,achieving a selectivity of 343.86 and a distribution coefficient of 36.66 for MeOH—significantly higher than[PMIM][H_(2)PO_(4)]and[BMIM][H_(2)PO_(4)].The accuracy of the LLE data was verified by Othmer–Tobias and Hand equations(R^(2)>0.90).The non-random two liquid model was used to correlate the experimental data(RMSD<2%).Besides,the combination of electrostatic surfaces potential,independent gradient model based on Hirshfeld partition,mean square displacement and radial distribution functions revealed strong electrostatic interactions between[H_(2)PO_(4)]^(–) and MeOH.Interaction energy analysis further emphasizes the mechanism of MeOH separation from a mixture of 2-MF and MeOH by ILs.This work provides a multiscale strategy for the separation of 2-MF and MeOH azeotropes,highlighting the potential of ILs to improve biofuel purification while reducing energy and environmental costs.展开更多
As the global textile industry has accelerated its transition to a circular economy,iterative innovation in regenerated cellulose fibers has become a key industry focus.With viscose fiber having been industrialized fo...As the global textile industry has accelerated its transition to a circular economy,iterative innovation in regenerated cellulose fibers has become a key industry focus.With viscose fiber having been industrialized for over a century and lyocell fiber gaining market recognition because of its environmentally friendly process,which is the next regenerated cellulose fiber.Herein,ionic liquids with low vapor pressure,nonflammability,relatively simple recovery,and high dissolution efficiency were used to fabricate regenerated cellulose fibers.The viscose and lyocell properties of the fibers were systematically compared,including microscopic morphology,dyeing behavior,fibrillation resistance,mechanical properties,yarn-forming capacity,and fabric performance.The ionic liquid(IL)fiber exhibited a smooth surface and circular cross-section,with the highest tensile strength,moderate dyeing and fibrillation properties,and similar spinning and weaving performance.This work can provide a reference for the commercial application of regenerated cellulose fibers fabricated from ionic liquid.展开更多
The preparation of ionic liquid gel electrolyte can reduce the occurrence of side effects and extend battery life.In the DMSO-ILZE electrolyte composed of DMSO,1-ethyl-3-methylimidazole tetrafluoroborate(EMIMBF_(4))an...The preparation of ionic liquid gel electrolyte can reduce the occurrence of side effects and extend battery life.In the DMSO-ILZE electrolyte composed of DMSO,1-ethyl-3-methylimidazole tetrafluoroborate(EMIMBF_(4))and Zn(BF_(4))_(2),the supramolecular gelatorβ-cyclodextrin(β-CD)was added,and then a gel electrolyte(CD-ILZE)for zinc-ion batteries was prepared through host-vip interaction betweenβ-CD and DMSO-ILZE electrolyte.The gel electrolyte has good conductivity between-30 and 80℃,which is found by fitting the Arrhenius equation that the gel electrolyte satisfies the liquid law within this temperature range.In addition,the supramolecular gel electrolyte can effectively decrease hydrogen evolution corrosion and the formation of zinc dendrites.Compared with the battery prepared by DMSO-ILZE electrolyte(about 1100 h),the prepared Zn||Zn battery exhibits a more stable cycle(over 2800 h)at a current density of 0.5 m A·cm^(-2).At 0.1 A·g^(-1),the prepared Zn||V_(2)O_(5)gel electrolyte cell has a capacity of 30 m Ah·g^(-1)and a capacity retention rate of 85.17%after more than 1500 cycles.The CD-ILZE supramolecular gel electrolyte can inhibit the formation of hydrogen evolution corrosion and zinc dendrites,and improve the cycling performance of the battery.展开更多
Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surf...Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.展开更多
Porous ionic liquid electrospray thrusters are the ideal propulsion technology for CubeSats because of their structural simplicity,high thrust accuracy and plume self-neutralization.The electrowetting technology can r...Porous ionic liquid electrospray thrusters are the ideal propulsion technology for CubeSats because of their structural simplicity,high thrust accuracy and plume self-neutralization.The electrowetting technology can replenish the propellant for the emitter online,thus prolonging the lifetime of the thruster.In order to gain a deeper understanding of its operating characteristics,the changes in thruster performance before and after propellant replenishment deserve to be scrutinized.In this study,the performance changes of a porous electrowetting ionic liquid electrospray thruster are tested by voltage-current test and time-of-flight mass spectrometry over a long operating time.The experimental results show that asymmetric operation with a negative current less than positive current for a long period of time causes anions to compensate for the emission after accumulation at the emitter,resulting in a phenomenon that the negative current is much larger than positive current.The reason for the difference in emission characteristics between the positive and negative modes is that the plume in the positive mode is quite ionized while the plume in the negative mode contains liquid droplets.This study provides a reference for the selection of operating conditions for ionic liquid electrospray thrusters.展开更多
Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,c...Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,classical molecular dynamics simulations struggle to accurately describe the complex interactions in ILs using the existing parameterized force fields.Recently,the MD simulations based on machine learning force fields(MLFFs)trained by first-principles calculations have attracted considerable attentions due to their abilities to balance computational accuracy and efficiency.Herein,we report the Bayesian-based MLFFs which can be successfully applied in IL systems and accelerate MD simulation.The calculated atomic forces,structures,and vibrational behaviors were validated to match the accuracy of firstprinciples calculations.Properties of the imidazolium-based ILs,including density,self-diffusion coefficients,viscosity,and radial distribution functions were predicted at the extended scales.Z-bonds that describe the unique structures in ILs were analyzed and the influences of Cpositions,temperature,and solvent H2O on Z-bonding configurations were systematically investigated.Our results confirmed that MLFFs presented the strong feasibility to investigate the large and complex systems,especially to predict structures and properties of the ILs.And the procedure described for MLFFs provides valuable guidance for researchers who are studying ILs.展开更多
The synthesis of propylene carbonate(PC)from CO_(2) and propylene oxide(PO)is a typical gas-liquid biphasic system,where gas-liquid mass transfer efficiency significantly influences CO_(2) cycloaddition reactions.Here...The synthesis of propylene carbonate(PC)from CO_(2) and propylene oxide(PO)is a typical gas-liquid biphasic system,where gas-liquid mass transfer efficiency significantly influences CO_(2) cycloaddition reactions.Here,we proposed a microchannel reaction system for the CO_(2) cycloaddition reaction catalyzed by ionic liquid within an aqueous environment.The effect of liquid flow rate,temperature and residence time on gas-liquid flow pattern,catalytic performance and mass transfer were systematically investigated.The results revealed that the PC generation rate reached 560.11 mmol·ml^(−1)·h^(−1)at a 50 cm of flow distance under reaction conditions of 105℃,2.5 MPa,QG=176 ml·min^(−1) and QL=0.3 ml·min^(−1).Variations in mass transfer rate and reaction rate at different flow distances were experimentally studied.The reaction efficiency gradually decreased with increasing flow distance,which were attributed to the reduction of mass transfer caused by decreasing bubble velocity.Optimizing bubble velocity at an appropriate position enhanced reaction efficiency by improving mass transfer,achieving a 97.7%PC yield within 2.85 min.Furthermore,a kinetic model coupling intrinsic kinetics with gas-liquid mass transfer was developed for CO_(2) cycloaddition reaction.The kinetic model was applied to predict PC reaction rates in microchannel reactors at various temperatures and liquid flow rates,achieving an average relative error of 9.6%.展开更多
The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit e...The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit exceptional electrochemical stability and compatibility with electrode electrolyte interfaces(EEIs),two major challenges persist:(i)safety risks caused by excessive low-flash-point diluents,and(ii)insufficient understanding of how diluents modulate solvation structures.Herein,we introduce a low-diluent-content LCILE system composed of lithium bis(fluorosulfonyl)imide(LiFSI)salt,N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide(Pyr_(13)FSI)ionic liquid,and trifluoromethanesulfonate(TFS)diluent.The TFS diluent strengthens ion-ion interactions by lowering the dielectric constant of the electrolyte,resulting in the formation of a unique nanometric anion aggregates(N-AGGs)reinforced solvation structure.These large anionic clusters exhibit accelerated redox decomposition kinetics,facilitating the rapid formation of a thin,dense,and low-impedance EEI.Consequently,the Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)coin cell achieves 87.8%capacity retention over 300 cycles at 4.3 V,while a practical 1.4 Ah Li/NCM622 pouch cell retains 84.5%capacity after 80 cycles at 4.5 V.Furthermore,the electrolyte demonstrates exceptional safety,and 2 Ah Li metal pouch cells successfully pass rigorous nail penetration tests without any ignition or explosion.This work not only provides a design strategy for intrinsically safe and high-performance electrolytes but also highlights the critical role of anion cluster decomposition kinetics in shaping EEI formation.展开更多
The density, viscosity and conductivity of ionic liquids （ILs）, 1-octyl-3-methylimidazolium tetrafluoroborate （[omim][BF4]）, 1-octyl-3-methylimidazolium chloride （[omim][C1]）, 1-hexyl-3-methylimidazolium tetrafl...The density, viscosity and conductivity of ionic liquids （ILs）, 1-octyl-3-methylimidazolium tetrafluoroborate （[omim][BF4]）, 1-octyl-3-methylimidazolium chloride （[omim][C1]）, 1-hexyl-3-methylimidazolium tetrafluoroborate （[hmim] BF4]）, 1-hexyl- 3-methylimidazolium chloride （[hmim][C1]）, 1-hexyl-3-methylimidazolium hexafluorophosphate （[hmim][PF6]）, and the [omim][BF4] ＋ [omim][Cl], [hmim][BF4] ＋ [hmim][C1], and [hmim][PF6] ＋ [hmim][C1] binary mixtures were studied at dif- ferent temperatures. It was demonstrated that the densities of both the neat ILs and their mixtures varied linearly with temper- ature. The density sensitivity of a binary mixture is between those of the two components. The excess molar volumes （l/e） of [hmim][BF4] ＋ [hmim][C1] and [hmim][PF6] ＋ [hmim][C1] mixtures are positive in the whole composition range. For [omim][BF4] ＋ [omim][C1], the VE is also positive in the [omirn][C1]-rich region, but is negative in the [omim][BF4]-rich re- gion. The viscosity or conductivity of a mixture is in the intermediate of those of the two neat ILs. For all the neat ILs and the binary mixtures studied, the order of conductivity is opposite to that of the viscosity. The Vogel-Tammann-Fulcher （VTF） equations can be used to fit the viscosity and conductivity of all the neat ILs and the binary mixtures. The neat ILs and their mixtures obey the Fractional Walden Rule very well, and the values of the Walden slopes are all smaller than unit, indicating obvious ion associations in the neat ILs and the binary mixtures.展开更多
A series of novel polyethylene glycol-dicationic imidazolium-based ionic liquids(mPEG-ILs)were synthesized by facile quaternization reaction from various elaborately designed di-imidazoles and PEG,which were then stud...A series of novel polyethylene glycol-dicationic imidazolium-based ionic liquids(mPEG-ILs)were synthesized by facile quaternization reaction from various elaborately designed di-imidazoles and PEG,which were then studied as green plasticizers for sustainable polylactide(PLA)material.展开更多
The design of stable,efficient and processable bactericidal materials represents a significant challenge for combating multidrugresistant bacteria in a variety of engineering fields.Herein,we report a facile strategy ...The design of stable,efficient and processable bactericidal materials represents a significant challenge for combating multidrugresistant bacteria in a variety of engineering fields.Herein,we report a facile strategy for the preparation of hollow polymeric nanosphere(HPN)-supported imidazolium-based ionic liquids(denoted as HPN-ILs)with superior antimicrobial activities.HPNILs were tailored by moderate Friedel−Crafts polymerization followed by the sequential covalent bonding of imidazole and bromoalkene.The resultant HPN-ILs have uniform hollow spherical morphology,an adequate surface area,and excellent physicochemical stability.Furthermore,they are highly active against both Gram-positive and Gram-negative bacteria and exhibit typical time/dosage-dependent antibacterial activities.The rational combination of porous HPNs and antibacterial ILs to generate an all-in-one entity may open new avenues for the design and fabrication of efficient bacteriostatic agents.Moreover,HPN-ILs have good biocompatibility and can also be loaded onto diverse matrices,and thus could extend their practical bactericidal application in the potential biomedical-active field.展开更多
The separations of olefin/paraffin,aromatic/aliphatic hydrocarbons or olefin isomers using ionic liquids instead of volatile solvents have interested many researchers.Activity coefficientsγ∞at infinite dilution of a...The separations of olefin/paraffin,aromatic/aliphatic hydrocarbons or olefin isomers using ionic liquids instead of volatile solvents have interested many researchers.Activity coefficientsγ∞at infinite dilution of a solute in ionic liquid are generally used in the selection of solvents for extraction or extractive distillation.In fact,the measurement ofγ∞by gas-liquid chromatography is a speedy and cost-saving method.Activity coefficients at infinite dilution of hydrocarbon solutes,such as alkanes,hexenes,alkylben-zenes,styrene,in 1-allyl-3-methylimidazolium tetrafluorobo-rate([AMIM][BF4])and 1-butyl-3-methyl imidazolium hexafluorophosphate([BMIM][PF6]),1-isobutenyl-3-methylimidazolium tetrafluoroborate([MPMIM][BF4])and[MPMIM][BF4]-AgBF4 have been determined by gas-liquid chromatography using ionic liquids as stationary phase.The measurements were carried out at different temperatures from 298 to 318 K.The separating effects of these ionic liquids for alkanes/hexane,aliphatic hydrocarbons/benzene and hexene isomers have been discussed.The hydrophobic parameter,dipole element,frontier molecular orbital energy gap and hydration energy of these hydrocarbons were calculated with the PM3 semi-empirical quantum chemistry method.The quantitative relations among the computed structure para-meters and activity coefficients at infinite dilution were also developed.The experimental activity coefficient data are consistent with the correlated and predicted results using QSPR models.展开更多
基金This work was supported by the National Natural Science Foundation of China(No.21477121)and the Fundamental Research Funds for the Central Universities for the support of this work.The numerical calculations were performed on the super computing system in the Supercomputing Center at the University of Science and Technology of China.
文摘Due to the large number of ionic liquids(ILs)and their potential environmental risk,assessing the toxicity of ILs by ecotoxicological experiment only is insufficient.Quantitative structure-activity relationship(QSAR)has been proven to be a quick and effective method to estimate the viscosity,melting points,and even toxicity of ILs.In this work,the LC50 values of 30 imidazolium-based ILs were determined with Caenorhabditis elegans as a model animal.Four suitable molecular descriptors were selected on the basis of genetic function approximation algorithm to construct a QSAR model with an R^2 value of 0.938.The predicted lgLC50 in this work are in agreement with the experimental values,indicating that the model has good stability and predictive ability.Our study provides a valuable model to predict the potential toxicity of ILs with different sub-structures to the environment and human health.
文摘Most of the onshore and offshore oil and gas reservoirs are facing operational challenges due to high temperature and high salinity, thus requiring advanced techniques for realizing the ex- pected oil recovery with the use of specially designed chemicals. During oil and gas well development, completion fluids, which are solids-free liquids, are used to complete an oil or gas well. Completion flu- ids consisting of brines are primarily used for oil and gas well stabilization and are corrosive in nature. There is a need to develop additives to be added with completion fluids to address the corrosive nature. The present investigation involved the usage of two imidazolium ionic liquids （ILs） as corrosion inhibi- tors for mild steel in various completion brine （CaCI2, HCOOCs and ZnBr2） fluids. The study was per- formed using various techniques, such as, potentiodynamic polarization, weight loss measurements and exposure studies. All the above techniques showed promising results which indicated that the ILs as corrosion inhibitors used were of the mixed-type following both physisorption and chemisorption over the mild steel surface. Among the two inhibitors studied here, l-octyl-3-methyl imidazolium chlo- ride （[OMIM]^＋[CI]^-） with longer alkyl chain exhibited better inhibition efficiency and much lesser cor- rosion rate than 1-butyl-3-methyl imidazolium chloride （[BMIM]^＋[Ci]^-） with a shorter alkyl chain. The results obtained from various methodologies indicate that ionic liquids can be explored to develop anti-corrosive completion fluids suitable for oil and gas reservoirs.
基金supported by the National Key R&D Program of China(2018YFB0605804)the National Natural Science Foundation of China(21606237)+2 种基金the Transformational Technologies for Clean Energy and Demonstration,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 21030500)the Fund of State Key Laboratory of Multiphase Complex Systems,IPE,CAS(MPCS-2019-A-02)the DNL Cooperation Fund,CAS(DNL180202)。
文摘The separation of methanol(MeOH)and dimethyl carbonate(DMC)is important but difficult due to the formation of an azeotropic mixture.In this work,isobaric vapor–liquid equilibrium(VLE)data for the ternary systems containing different imidazolium–based ionic liquids(ILs),i.e.MeOH+DMC+1-butyl-3-methy-limidazolium bis[(trifluoromethyl)sulfonyl]imide([Bmim][Tf2N]),MeOH+DMC+1-ethyl-3-methyl-imidazolium bis[(trifluoromethyl)sulfonyl]imide([Emim][Tf2N]),and MeOH+DMC+1-ethyl-3-methylimidazolium hexafluorophosphate([Emim][PF6])were measured at 101.3 kPa.The mole fraction of IL was varied from0.05 to 0.20.The experimental data were correlated with the NRTL and Wilson equations,respectively.The results show that imidazolium-based ILs were beneficial to improve the relative volatility of MeOH to DMC,and[Bmim][Tf2 N]showed a much more excellent performance on the activity coefficient of MeOH.The interaction energies of system components were calculated using Gaussian program,and the effects of cation and anion on the separation coefficient of the azeotropic system were discussed.
基金Supported by the National Natural Science Foundation of China(21076126)the Program for Liaoning Excellent Talents in University(2012013)the Liaoning Province Science Foundation of China(2014020140)
文摘Three ionic liquids(ILs),1-ethyl-3-methylimidazolium bromine([EMIM]Br),1-butyl-3-methylimidazolium bromine([BMIM]Br),and 1-hexyl-3-methylimidazolium bromine([HMIM]Br),were used as the solvent for separation of {tert-butyl alcohol(TBA)+ water} azeotrope.Vapor–liquid equilibrium(VLE)data for {TBA + water + IL}ternary systems were measured at 101.3 k Pa.The results indicate that all the three ILs produce an obvious effect on the VLE behavior of {TBA + water} system and eliminate the azeotropy in the whole concentration range.[EMIM]Br is the best solvent for the separation of {TBA + water} system by extractive distillation among the three ILs.The experimental VLE data for the ternary systems are correlated with the NRTL model equation with good correlations.Explanations are given with activity coefficients of water and TBA,and the experimental VLE-temperature data for {TBA or water + IL} binary systems.
基金financial support from the National Science Fund for Excellent Young Scholars(21722610)Taishan Scholars Program of Shandong Province(tsqn201909091)。
文摘How to completely remove the water from ionic liquids(ILs)is difficult for researchers because of the hygroscopicity of ILs.In order to study the hygroscopicity of ILs,two kinds of ILs,1-Butyl-3-methylimidazolium hexafluorophosphate([Bmim][PF6])and 1-Butyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)([Bmim][NTf_(2)])were investigated by molecular dynamics simulations.Although[Bmim][PF6]and[Bmim][NTf_(2)]are hydrophobic,both of the ILs could absorb water molecules from the vapor.In this work,the process of absorbing water from the vapor phase was studied,and the water molecules could disperse into the IL.Aggregation was observed with increasing the water concentration.Although the absorbed water increases obviously,the amount of free water and small cluster in the ILs does not change significantly and always stays at a certain level.The amount of free water and small cluster in[Bmim][PF6]is more than that in[Bmim][NTf_(2)],which is consistent with their hydrophobicity.In addition,the liquid-vacuum and liquid–liquid interfaces of the ILs were simulated and analyzed in detail.The number density distribution and angle distribution indicated that[Bmim]+cations arrangement regularly at the IL-vacuum interface.The butyl chain point to the vacuum,while the imidazlium ring is close to the IL phase region and perpendicular to the interface.While at the IL-water interface,the cations and anions are disordered.
基金support from the National Natural Science Foundation of China(62074095)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities(GK202002001)the 111 Project(Grant No.B21005)the DNL Cooperation Fund CAS(DNL180311)the support of H2 cluster in Xi’an Jiaotong University.
文摘The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.
文摘The interactions of bovine serum albumin (BSA) with two alkylimidazolium-based ionic liquids, 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim]BF4) and 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim]PF6), in buffer solutions at pH 7.0 were investigated by isothermal titration calorimetry (ITC) and circular dichroism (CD). CD spectra showed that the two ionic liquids changed the secondary structure of BSA. Data process was based on the supposition that there were several independent types of binding sites on each BSA molecule for the two ligand molecules. The results obtained by using this supposition combined with Langmuir adsorption model showed that there were two types of such binding sites. One was the high affinity binding site, and the other was the low affinity binding site. The binding constants, changes in enthalpy, entropy and Gibbs free energy for the two types of binding were obtained, which showed that the two types of binding were driven by a favorable entropy increase. Furthermore, for either the ionic liquids, the number of the high affinity binding sites is much smaller than that of the low affinity ones. These results were interpreted with the molecular structure of BSA and the different substituent groups on imidazole ring of the two ionic liquid molecules.
文摘In this work,we proposed a strategy for the hydrolysis of native corn starch after the treatment of corn starch in an ionic liquid aqueous solution,and it is an awfully“green”and simple means to obtain starch with low molecular weight and amorphous state.X-ray diffraction results revealed that the natural starch crystalline region was largely disrupted by ionic liquid owing to the broken intermolecular and intramolecular hydrogen bonds.After hydrolysis,the morphology of starch changed from particles of native corn starch into little pieces,and their molecular weight could be effectively regulated during the hydrolysis process,and also the hydrolyzed starch samples exhibited decreased thermal stability with the extension of hydrolysis time.This work would counsel as a powerful tool for the development of native starch in realistic applications.
基金supported by the National Natural Science Foundation of China(22278272)Natural Science Foundation of Liaoning Province(2024-MS-129).
文摘Separation of 2-methylfuran(2-MF)and methanol(MeOH)azeotropes is a key challenge in biofuel production because of the efficiency and sustainability issues of conventional methods.In this study,ionic liquids(ILs)were introduced as green solvents for separation of 2-MF/MeOH through liquid–liquid equilibrium(LLE)experiment.Three ILs,namely 1-ethyl-3-methylimidazole dihydrogen phosphate([EMIM][H_(2)PO_(4)]),1-propyl-3-methylimidazole dihydrogen phosphate([PMIM][H_(2)PO_(4)])and 1-butyl-3-methylimidazole dihydrogen phosphate([BMIM][H_(2)PO_(4)]),were screened out from 425 candidates using the conductor-like screening model for real solvents(COSMO-RS).Then,the ternary LLE data of 2-MF(1)+MeOH(2)+ILs(3)were determined at 30℃ and 101.32 kPa.Results confirmed[EMIM][H_(2)PO_(4)]as the best performer,achieving a selectivity of 343.86 and a distribution coefficient of 36.66 for MeOH—significantly higher than[PMIM][H_(2)PO_(4)]and[BMIM][H_(2)PO_(4)].The accuracy of the LLE data was verified by Othmer–Tobias and Hand equations(R^(2)>0.90).The non-random two liquid model was used to correlate the experimental data(RMSD<2%).Besides,the combination of electrostatic surfaces potential,independent gradient model based on Hirshfeld partition,mean square displacement and radial distribution functions revealed strong electrostatic interactions between[H_(2)PO_(4)]^(–) and MeOH.Interaction energy analysis further emphasizes the mechanism of MeOH separation from a mixture of 2-MF and MeOH by ILs.This work provides a multiscale strategy for the separation of 2-MF and MeOH azeotropes,highlighting the potential of ILs to improve biofuel purification while reducing energy and environmental costs.
基金financially supported by the National Natural Science Foundation of China(Nos.22005226 and 52203124)Center for Carbon Neutral Chemistry,Institute of Chemistry,Chinese Academy of Sciences(No.CCNC-202402)+1 种基金the Basic and Advanced Research Project from Wuhan Science and Technology Bureau(No.2022013988065201)Hubei Integrative Technology and Innovation Center for Advanced Fiberous Materials,project(No.XC2024G3013)。
文摘As the global textile industry has accelerated its transition to a circular economy,iterative innovation in regenerated cellulose fibers has become a key industry focus.With viscose fiber having been industrialized for over a century and lyocell fiber gaining market recognition because of its environmentally friendly process,which is the next regenerated cellulose fiber.Herein,ionic liquids with low vapor pressure,nonflammability,relatively simple recovery,and high dissolution efficiency were used to fabricate regenerated cellulose fibers.The viscose and lyocell properties of the fibers were systematically compared,including microscopic morphology,dyeing behavior,fibrillation resistance,mechanical properties,yarn-forming capacity,and fabric performance.The ionic liquid(IL)fiber exhibited a smooth surface and circular cross-section,with the highest tensile strength,moderate dyeing and fibrillation properties,and similar spinning and weaving performance.This work can provide a reference for the commercial application of regenerated cellulose fibers fabricated from ionic liquid.
文摘The preparation of ionic liquid gel electrolyte can reduce the occurrence of side effects and extend battery life.In the DMSO-ILZE electrolyte composed of DMSO,1-ethyl-3-methylimidazole tetrafluoroborate(EMIMBF_(4))and Zn(BF_(4))_(2),the supramolecular gelatorβ-cyclodextrin(β-CD)was added,and then a gel electrolyte(CD-ILZE)for zinc-ion batteries was prepared through host-vip interaction betweenβ-CD and DMSO-ILZE electrolyte.The gel electrolyte has good conductivity between-30 and 80℃,which is found by fitting the Arrhenius equation that the gel electrolyte satisfies the liquid law within this temperature range.In addition,the supramolecular gel electrolyte can effectively decrease hydrogen evolution corrosion and the formation of zinc dendrites.Compared with the battery prepared by DMSO-ILZE electrolyte(about 1100 h),the prepared Zn||Zn battery exhibits a more stable cycle(over 2800 h)at a current density of 0.5 m A·cm^(-2).At 0.1 A·g^(-1),the prepared Zn||V_(2)O_(5)gel electrolyte cell has a capacity of 30 m Ah·g^(-1)and a capacity retention rate of 85.17%after more than 1500 cycles.The CD-ILZE supramolecular gel electrolyte can inhibit the formation of hydrogen evolution corrosion and zinc dendrites,and improve the cycling performance of the battery.
基金supported by the Research Projects of the Department of Education of Guangdong Province 2024ZDZX3079The financial support from the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011677)+4 种基金the Scientific and Technical Innovation Council of Shenzhen(20220812165832002)the Research Projects of Department of Education of Guangdong Province-2023GCZX015the Innovation Team Project of Guangdong(2022KCXTD055)the China Postdoctoral Science Foundation(Certificate Number:2024M763441)is gratefully acknowledgedsupported by the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20250031 and Research Projects of the Department of Education of Guangdong Province 2023GCZX015。
文摘Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.
基金co-supported by the National Key R&D Program of China(Nos.2020YFC2201103 and 2022YFB4601300)the National Natural Science Foundation of China(No.U22B20120)+1 种基金the Program of Beijing Engineering Research Center of Efficient and Green Aerospace Propulsion Technology,China(No.Lab ASP-2024-09)the Beijing Institute of Technology Research Fund Program for Young Scholars,China。
文摘Porous ionic liquid electrospray thrusters are the ideal propulsion technology for CubeSats because of their structural simplicity,high thrust accuracy and plume self-neutralization.The electrowetting technology can replenish the propellant for the emitter online,thus prolonging the lifetime of the thruster.In order to gain a deeper understanding of its operating characteristics,the changes in thruster performance before and after propellant replenishment deserve to be scrutinized.In this study,the performance changes of a porous electrowetting ionic liquid electrospray thruster are tested by voltage-current test and time-of-flight mass spectrometry over a long operating time.The experimental results show that asymmetric operation with a negative current less than positive current for a long period of time causes anions to compensate for the emission after accumulation at the emitter,resulting in a phenomenon that the negative current is much larger than positive current.The reason for the difference in emission characteristics between the positive and negative modes is that the plume in the positive mode is quite ionized while the plume in the negative mode contains liquid droplets.This study provides a reference for the selection of operating conditions for ionic liquid electrospray thrusters.
基金supported by the National Natural Science Foundation of China(Nos.22278397)the Fundamental Research Funds for the Central Universities(2024SMECP01).
文摘Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,classical molecular dynamics simulations struggle to accurately describe the complex interactions in ILs using the existing parameterized force fields.Recently,the MD simulations based on machine learning force fields(MLFFs)trained by first-principles calculations have attracted considerable attentions due to their abilities to balance computational accuracy and efficiency.Herein,we report the Bayesian-based MLFFs which can be successfully applied in IL systems and accelerate MD simulation.The calculated atomic forces,structures,and vibrational behaviors were validated to match the accuracy of firstprinciples calculations.Properties of the imidazolium-based ILs,including density,self-diffusion coefficients,viscosity,and radial distribution functions were predicted at the extended scales.Z-bonds that describe the unique structures in ILs were analyzed and the influences of Cpositions,temperature,and solvent H2O on Z-bonding configurations were systematically investigated.Our results confirmed that MLFFs presented the strong feasibility to investigate the large and complex systems,especially to predict structures and properties of the ILs.And the procedure described for MLFFs provides valuable guidance for researchers who are studying ILs.
基金supported by the National Key Projects for Fundamental Research and development of China(2020YFA0710202)the China Postdoctoral Science Foundation(2024M761567)Shandong Postdoctoral Science Foundation(SDCX-ZG-202400271).
文摘The synthesis of propylene carbonate(PC)from CO_(2) and propylene oxide(PO)is a typical gas-liquid biphasic system,where gas-liquid mass transfer efficiency significantly influences CO_(2) cycloaddition reactions.Here,we proposed a microchannel reaction system for the CO_(2) cycloaddition reaction catalyzed by ionic liquid within an aqueous environment.The effect of liquid flow rate,temperature and residence time on gas-liquid flow pattern,catalytic performance and mass transfer were systematically investigated.The results revealed that the PC generation rate reached 560.11 mmol·ml^(−1)·h^(−1)at a 50 cm of flow distance under reaction conditions of 105℃,2.5 MPa,QG=176 ml·min^(−1) and QL=0.3 ml·min^(−1).Variations in mass transfer rate and reaction rate at different flow distances were experimentally studied.The reaction efficiency gradually decreased with increasing flow distance,which were attributed to the reduction of mass transfer caused by decreasing bubble velocity.Optimizing bubble velocity at an appropriate position enhanced reaction efficiency by improving mass transfer,achieving a 97.7%PC yield within 2.85 min.Furthermore,a kinetic model coupling intrinsic kinetics with gas-liquid mass transfer was developed for CO_(2) cycloaddition reaction.The kinetic model was applied to predict PC reaction rates in microchannel reactors at various temperatures and liquid flow rates,achieving an average relative error of 9.6%.
基金supported by the National Key R&D Program of China(Grant No.2022YFE0207300)the National Natural Science Foundation of China(Grant Nos.22179142 and 22075314)+1 种基金Jiangsu Provincial Science and Technology Program(Grant No.BG 2024020).XPSWAXS and TOF-SIMS characterizations were supported by Nano-X(Vacuum Interconnected Nanotech Workstation,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO),Suzhou 215123,China)。
文摘The practical application of lithium metal batteries(LMBs)requires electrolytes that simultaneously ensure high safety and interfacial stability.Although locally concentrated ionic liquid electrolytes(LCILEs)exhibit exceptional electrochemical stability and compatibility with electrode electrolyte interfaces(EEIs),two major challenges persist:(i)safety risks caused by excessive low-flash-point diluents,and(ii)insufficient understanding of how diluents modulate solvation structures.Herein,we introduce a low-diluent-content LCILE system composed of lithium bis(fluorosulfonyl)imide(LiFSI)salt,N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide(Pyr_(13)FSI)ionic liquid,and trifluoromethanesulfonate(TFS)diluent.The TFS diluent strengthens ion-ion interactions by lowering the dielectric constant of the electrolyte,resulting in the formation of a unique nanometric anion aggregates(N-AGGs)reinforced solvation structure.These large anionic clusters exhibit accelerated redox decomposition kinetics,facilitating the rapid formation of a thin,dense,and low-impedance EEI.Consequently,the Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)coin cell achieves 87.8%capacity retention over 300 cycles at 4.3 V,while a practical 1.4 Ah Li/NCM622 pouch cell retains 84.5%capacity after 80 cycles at 4.5 V.Furthermore,the electrolyte demonstrates exceptional safety,and 2 Ah Li metal pouch cells successfully pass rigorous nail penetration tests without any ignition or explosion.This work not only provides a design strategy for intrinsically safe and high-performance electrolytes but also highlights the critical role of anion cluster decomposition kinetics in shaping EEI formation.
基金supported by the National Natural Science Foundation of China (21133009, 21073207, 20903109)
文摘The density, viscosity and conductivity of ionic liquids （ILs）, 1-octyl-3-methylimidazolium tetrafluoroborate （[omim][BF4]）, 1-octyl-3-methylimidazolium chloride （[omim][C1]）, 1-hexyl-3-methylimidazolium tetrafluoroborate （[hmim] BF4]）, 1-hexyl- 3-methylimidazolium chloride （[hmim][C1]）, 1-hexyl-3-methylimidazolium hexafluorophosphate （[hmim][PF6]）, and the [omim][BF4] ＋ [omim][Cl], [hmim][BF4] ＋ [hmim][C1], and [hmim][PF6] ＋ [hmim][C1] binary mixtures were studied at dif- ferent temperatures. It was demonstrated that the densities of both the neat ILs and their mixtures varied linearly with temper- ature. The density sensitivity of a binary mixture is between those of the two components. The excess molar volumes （l/e） of [hmim][BF4] ＋ [hmim][C1] and [hmim][PF6] ＋ [hmim][C1] mixtures are positive in the whole composition range. For [omim][BF4] ＋ [omim][C1], the VE is also positive in the [omirn][C1]-rich region, but is negative in the [omim][BF4]-rich re- gion. The viscosity or conductivity of a mixture is in the intermediate of those of the two neat ILs. For all the neat ILs and the binary mixtures studied, the order of conductivity is opposite to that of the viscosity. The Vogel-Tammann-Fulcher （VTF） equations can be used to fit the viscosity and conductivity of all the neat ILs and the binary mixtures. The neat ILs and their mixtures obey the Fractional Walden Rule very well, and the values of the Walden slopes are all smaller than unit, indicating obvious ion associations in the neat ILs and the binary mixtures.
基金The authors are grateful for financial support from the National Natural Science Foundation of China(No.51573130)the Open Foundation of Beijing Key Laboratory of Quality Evaluation Tech no logy for Hygiene and Safety of Plastics.
文摘A series of novel polyethylene glycol-dicationic imidazolium-based ionic liquids(mPEG-ILs)were synthesized by facile quaternization reaction from various elaborately designed di-imidazoles and PEG,which were then studied as green plasticizers for sustainable polylactide(PLA)material.
基金supported by the Shanghai Sailing Program(No.21YF1431000)I.K.thanks to the National Research Foundation of Korea grant funded by the Korean government(MSIT)(No.2021R1A2C2003685)for financial support.
文摘The design of stable,efficient and processable bactericidal materials represents a significant challenge for combating multidrugresistant bacteria in a variety of engineering fields.Herein,we report a facile strategy for the preparation of hollow polymeric nanosphere(HPN)-supported imidazolium-based ionic liquids(denoted as HPN-ILs)with superior antimicrobial activities.HPNILs were tailored by moderate Friedel−Crafts polymerization followed by the sequential covalent bonding of imidazole and bromoalkene.The resultant HPN-ILs have uniform hollow spherical morphology,an adequate surface area,and excellent physicochemical stability.Furthermore,they are highly active against both Gram-positive and Gram-negative bacteria and exhibit typical time/dosage-dependent antibacterial activities.The rational combination of porous HPNs and antibacterial ILs to generate an all-in-one entity may open new avenues for the design and fabrication of efficient bacteriostatic agents.Moreover,HPN-ILs have good biocompatibility and can also be loaded onto diverse matrices,and thus could extend their practical bactericidal application in the potential biomedical-active field.
基金supported by the Science Foundation of China Petroleum&Chemical Corporation(Grant No.X504031).
文摘The separations of olefin/paraffin,aromatic/aliphatic hydrocarbons or olefin isomers using ionic liquids instead of volatile solvents have interested many researchers.Activity coefficientsγ∞at infinite dilution of a solute in ionic liquid are generally used in the selection of solvents for extraction or extractive distillation.In fact,the measurement ofγ∞by gas-liquid chromatography is a speedy and cost-saving method.Activity coefficients at infinite dilution of hydrocarbon solutes,such as alkanes,hexenes,alkylben-zenes,styrene,in 1-allyl-3-methylimidazolium tetrafluorobo-rate([AMIM][BF4])and 1-butyl-3-methyl imidazolium hexafluorophosphate([BMIM][PF6]),1-isobutenyl-3-methylimidazolium tetrafluoroborate([MPMIM][BF4])and[MPMIM][BF4]-AgBF4 have been determined by gas-liquid chromatography using ionic liquids as stationary phase.The measurements were carried out at different temperatures from 298 to 318 K.The separating effects of these ionic liquids for alkanes/hexane,aliphatic hydrocarbons/benzene and hexene isomers have been discussed.The hydrophobic parameter,dipole element,frontier molecular orbital energy gap and hydration energy of these hydrocarbons were calculated with the PM3 semi-empirical quantum chemistry method.The quantitative relations among the computed structure para-meters and activity coefficients at infinite dilution were also developed.The experimental activity coefficient data are consistent with the correlated and predicted results using QSPR models.
