Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within...Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within less than 30 min under mild conditions.展开更多
Stable silver nanoparticles was successfully synthesized by chemical reduction of silver nitrate in an ionic liquid,1-n-butyl-3-methylimidazolium tetrafluoroborate（[BMIM]·BF4） at room temperature.Results of UV-...Stable silver nanoparticles was successfully synthesized by chemical reduction of silver nitrate in an ionic liquid,1-n-butyl-3-methylimidazolium tetrafluoroborate（[BMIM]·BF4） at room temperature.Results of UV-Vis diffuse reflectance spectroscopy show as-prepared Ag nanoparticles exhibit a typical emission peak at 400―430 nm.By varying the reaction temperature and the precursor concentration,the size and the shape of the silver nanoparticles could be easily controlled under mild conditions.Analyses of transmission electron micrographs,X-ray diffraction pattern and X-ray photoelectron spectrum further reveal that the silver nanoparticles were coated incompletely by [BMIM]·BF4.Microbial experiments indicate that as-prepared silver nanoparticles show a wide spectrum of antimicrobial activities and have better antimicrobial activities to Pseudomonas aeruginosa than silver nitrate with the same concentration of silver.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
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
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
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
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
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
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
Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-...Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.展开更多
A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic syn...A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic synthesis of cyclic carbonates and oxazolidinones via the cycloaddition reactions between CO_(2) and epoxides or aziridines with excellent yield and high selectivity in the absence of co-catalyst,metal and solvent.Due to the synergistic effects of hydroxyl groups and halogen anion,the cycloaddition reactions proceeded smoothly either at atmospheric pressure or room temperature.The selectivity for substituted oxazolidinones at 5-and 4-positions can be tuned via changing the reaction conditions.Finally,possible mechanisms including the activation of both CO_(2) and epoxide or aziridines were proposed based on the literatures and experimental results.展开更多
The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel ap...The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.展开更多
Electrochemical reduction of CO_(2)is a promising approach to convert CO_(2)to high-valued chemicals and fuels.However,developing efficient electrocatalysts featuring desirable activity and selectivity is still a big ...Electrochemical reduction of CO_(2)is a promising approach to convert CO_(2)to high-valued chemicals and fuels.However,developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge.In this work,a strategy of introducing functionalized molecules with desirable CO_(2)affinity to regulate Ag catalyst for promoting electrochemical reduction of CO_(2)was proposed.Specifically,3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle(Ag-m-Triz)for the first time to achieve selectively converting CO_(2)to carbon monoxide(CO).This Ag-m-Triz exhibits excellent performance for CO_(2)reduction with a high CO Faradaic efficiency(FECO)of 99.2%and CO partial current density of 85.0 mA cm^(-2)at-2.3 V vs.Ag/Ag^(+) in H-cell when combined with the ionic liquid-based electrolyte,30 wt%1-butyl-3-methylimidazolium hexafluorophosphate([Bmim][PF6])-65 wt%acetonitrile(AcN)-5 wt%H2O,which is 2.5-fold higher than the current density in Ag-powder under the same condition.Mechanism studies confirm that the significantly improved performance of Ag-m-Triz originates from(i)the stronger adsorption ability of CO_(2)molecule and(ii)the weaker binding energy to form the COOH*intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst,which boosts the conversion of CO_(2)to CO.This research provides a facile way to regulate electrocatalysts for efficient CO_(2)reduction by introducing functionalized molecules.展开更多
A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+)...A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+).Characterization of the materials was carried out using techniques such as X-ray diffraction(XRD),Fourier transform infrared(FTIR),scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS),thermogravimetric analysis(TGA)and Brunauer-Emmett-Teller(BET).The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and mo rphology of MIL-101(Cr).Adsorption experiments were conducted to explore parameters including equilibrium pH,initial Eu3+concentration,and duration,with comprehensive analyses of adsorption kinetics,isotherms,and mechanisms.Findings reveal that Poly(IL1-AA)@MIL-101(Cr),Poly(IL3-AA)@MIL-101(Cr),and Poly(IL5-AA)@MIL-101(Cr)achieve adsorption equilibrium for Eu3+at approximately 9 h with an equilibrium pH of 6.2.The adso rption of Eu^(3+)predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model.Moreover,the prepared composite material exhibits superior adsorption selectivity for Eu^(3+)over other metal ions in the mixture(K^(+),Mg^(2+),Ni^(2+),Co^(2+),Zn^(2+),La^(3+),and Nd^(3+)).Even after five adsorption-desorption cycles,the composite material maintains satis factory adsorption performance.展开更多
The composite membrane of microcrystalline cellulose(MCC)with polyvinyl alcohol(PVA)was effectively synthesized using ionic liquids(ILs)as the solvent and dimethyl sulfone(DMSO)as the co-solvent through the phase conv...The composite membrane of microcrystalline cellulose(MCC)with polyvinyl alcohol(PVA)was effectively synthesized using ionic liquids(ILs)as the solvent and dimethyl sulfone(DMSO)as the co-solvent through the phase conversion method.The effects of IL structure and the IL/DMSO mass ratio on the solubility of MCC were investigated.The findings indicated that the composite solvent functioned as a non-derivative solvent for MCC dissolution.The inclusion of DMSO decreased the viscosity of ILs and enhanced the rate of MCC dissolution.The solubility of MCC reached 14.5%(mass)when the mass ratio of[Bmim]Cl to DMSO was 1:1.The fabricated MCC membrane exhibited a smooth surface and a dense structure.PVA@MCC demonstrated exceptional mechanical properties and a uniform structure at a mass ratio of 2:1,with an elongation at break of 76%and a tensile strength of 14.6 MPa.The effects of antibacterial agents on the morphology,transmittance,mechanical properties,and antibacterial efficiency of PVA@MCC were investigated.The findings revealed that PVA@MCC fortified with clove oil showcased a flat and smooth surface,devoid of stratification or aggregation,and demonstrated superior mechanical properties compared to its counterparts with chitosan and ZnO additions.The elongation at break of PVA@MCC with clove oil increased to 137.6%,while its tensile strength decreased to 10.4 MPa.PVA@MCC with clove oil exhibited an antibacterial efficiency exceeding 68%against Escherichia coli,Staphylococcus aureus,and Pseudomonas aeruginosa,thereby extending the shelf life of cherry tomatoes by an additional four days at ambient temperature.展开更多
The recovery of ionic liquids(ILs)has attracted growing attention as an indispensable process in“green”industrial applications.Forward osmosis(FO)has proven to be a sustainable method for concentrating the very dilu...The recovery of ionic liquids(ILs)has attracted growing attention as an indispensable process in“green”industrial applications.Forward osmosis(FO)has proven to be a sustainable method for concentrating the very dilute aqueous solutions of ILs at ambient temperature,in which semi-permeable membranes play a vital role in determining the recovery efficiency.Herein,we use interfacial polymerization method to prepare thin-film composite membranes consisting of polyamide skin layer and electrospun nanofibrous substrate with tunable water permeability and IL selectivity for osmotic enrichment of imidazolium ILs from their dilute aqueous solutions through FO process.The resulting FO membrane shows a compact polyamide layer with a thickness of 30-200 nm,guranteeing a high selectivity to ILs and water.Meanwhile,the nanofibrous substrate with large and interconnect pores as well as low tortuosity,providing mechanical and permeable support for the composite membranes.IL structure influences the osmotic pressure difference as well as the interactions with polyamide layer of the membrane and thus determines the whole concentration process.First,the alkyl chain growth augments the osmosis pressure difference between the ILs solution and draw solution,resulting in an enhancement in driving force of water osmosis and IL enrichment.Moreover,alkyl length aggravates external concentration polarization caused by the enhanced adsorption of ILs onto the skin layer via electrostatic and alkyl-πinteractions.Meanwhile,such adsorbed ILs further enhance the IL retention but decrease the reverse salt diffusion.Therefore,imidazolium ILs with varied alkyl lengths are ultimately enriched with a 100-fold increase in concentration from their dilute aqueous solutions with high IL/NaCl rejection and low IL loss.Remarkably,the final concentration of IL with longest alkyl length reaches the highest(6.4 mol·L^(-1)).This work provides the insights in respect to material preparation and process amelioration for IL recovery with high scalability at mild conditions.展开更多
Flammable ionic liquids exhibit high conductivity and a broad electrochemical window,enabling the generation of combustible gases for combustion via electrochemical decomposition and thermal decomposition.This charact...Flammable ionic liquids exhibit high conductivity and a broad electrochemical window,enabling the generation of combustible gases for combustion via electrochemical decomposition and thermal decomposition.This characteristic holds significant implications in the realm of novel satellite propulsion.Introducing a fraction of the electrical energy into energetic ionic liquid fuels,the thermal decomposition process is facilitated by reducing the apparent activation energy required,and electrical energy can trigger the electrochemical decomposition of ionic liquids,presenting a promising approach to enhance combustion efficiency and energy release.This study applied an external voltage during the thermal decomposition of 1-ethyl-3-methylimidazole nitrate([EMIm]NO_(3)),revealing the effective alteration of the activation energy of[EMIm]NO_(3).The pyrolysis,electrochemical decomposition,and electron assisted enhancement products were identified through Thermogravimetry-Differential scanning calorimetry-Fourier transform infrared-Mass spectrometry(TG-DSC-FTIR-MS)and gas chromatography(GC)analyses,elucidating the degradation mechanism of[EMIm]NO_(3).Furthermore,an external voltage was introduced during the combustion of[EMIm]NO_(3),demonstrating the impact of voltage on the combustion process.展开更多
Silver still faces significant challenges in the electrochemical reduction of CO_(2)(eCO_(2)RR)to CO under elevated current density with high energy input due to the intensified hydrogen evolution reaction.The doping ...Silver still faces significant challenges in the electrochemical reduction of CO_(2)(eCO_(2)RR)to CO under elevated current density with high energy input due to the intensified hydrogen evolution reaction.The doping of 2 mol%Re-oxide into Ag aerogel results in a significant decrease in the onset potential and a twofold increase in the current density compared to a pure Ag aerogel(Ag100),which tackles the issue.The effect is rationalized in terms of positively shifting the d-band center close to the Fermi energy level to change the density of local electronic states.Moreover,upon the adsorption of the ionic liquid(IL,1-Allyl-3-methylimidazolium dicyanamide[AMIM][DCN])onto the surface of Re-oxide doped Ag aerogel(Ag_(98)Re_(2)/IL),the current density increases to 320 mA/cm^(2) at a low of-1.3 V vs.RHE with 96%selectivity for CO formation in an alkaline medium using a flow cell electrolyzer,and maintains the selectivity above92%for up to 17 h using an H-cell electrolyzer.Density Functional Theory revealed that the adsorbed IL forms a highly conductive and hydrophobic layer on the aerogel surface,presumably decreasing the local H+concentration,greatly suppressing the hydrogen evolution reaction while enhancing the eCO_(2)RR pathway and mitigating the mass transport issues typically associated with IL use.This work addressed the key challenges in massively producing CO from eCO_(2)RR,offering a promising strategy for scalable and industrial CO generation.展开更多
基金We thank the financial support from the National Natural Science Foundation of China.(No.20172038)
文摘Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within less than 30 min under mild conditions.
文摘Stable silver nanoparticles was successfully synthesized by chemical reduction of silver nitrate in an ionic liquid,1-n-butyl-3-methylimidazolium tetrafluoroborate（[BMIM]·BF4） at room temperature.Results of UV-Vis diffuse reflectance spectroscopy show as-prepared Ag nanoparticles exhibit a typical emission peak at 400―430 nm.By varying the reaction temperature and the precursor concentration,the size and the shape of the silver nanoparticles could be easily controlled under mild conditions.Analyses of transmission electron micrographs,X-ray diffraction pattern and X-ray photoelectron spectrum further reveal that the silver nanoparticles were coated incompletely by [BMIM]·BF4.Microbial experiments indicate that as-prepared silver nanoparticles show a wide spectrum of antimicrobial activities and have better antimicrobial activities to Pseudomonas aeruginosa than silver nitrate with the same concentration of silver.
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.
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 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.
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.
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 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sponsored by the National Natural Science Foundation of China (Nos. 22308145, 22208140, 22178159, 22078145)Natural Science Foundation of Jiangsu Province (BK20230791)Postgraduate Research Innovation Program of Jiangsu Province (KYCX24_0165)。
文摘Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.
文摘A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic synthesis of cyclic carbonates and oxazolidinones via the cycloaddition reactions between CO_(2) and epoxides or aziridines with excellent yield and high selectivity in the absence of co-catalyst,metal and solvent.Due to the synergistic effects of hydroxyl groups and halogen anion,the cycloaddition reactions proceeded smoothly either at atmospheric pressure or room temperature.The selectivity for substituted oxazolidinones at 5-and 4-positions can be tuned via changing the reaction conditions.Finally,possible mechanisms including the activation of both CO_(2) and epoxide or aziridines were proposed based on the literatures and experimental results.
基金financial support from the National Natural Science Foundation of China(Nos.22071222,22171249)the Natural Science Foundation of Henan Province(Nos.232300421363,242300420526)+2 种基金Key Research Projects of Universities in Henan Province(No.23A180010)Science&Technology Innovation Talents in Universities of Henan Province(No.23HASTIT003)Science and Technology Research and Development Plan Joint Fund of Henan Province(No.242301420006)。
文摘The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.
基金supported by the Swedish Energy Agency(P47500-1)the National Key R&D Program of China(2020YFA0710200)+2 种基金the National Natural Science Foundation of China(22378401 and U22A20416)the financial support from STINT(CH2019-8287)support from the European Union and Swedish Energy Agency(P2020-90066).
文摘Electrochemical reduction of CO_(2)is a promising approach to convert CO_(2)to high-valued chemicals and fuels.However,developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge.In this work,a strategy of introducing functionalized molecules with desirable CO_(2)affinity to regulate Ag catalyst for promoting electrochemical reduction of CO_(2)was proposed.Specifically,3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle(Ag-m-Triz)for the first time to achieve selectively converting CO_(2)to carbon monoxide(CO).This Ag-m-Triz exhibits excellent performance for CO_(2)reduction with a high CO Faradaic efficiency(FECO)of 99.2%and CO partial current density of 85.0 mA cm^(-2)at-2.3 V vs.Ag/Ag^(+) in H-cell when combined with the ionic liquid-based electrolyte,30 wt%1-butyl-3-methylimidazolium hexafluorophosphate([Bmim][PF6])-65 wt%acetonitrile(AcN)-5 wt%H2O,which is 2.5-fold higher than the current density in Ag-powder under the same condition.Mechanism studies confirm that the significantly improved performance of Ag-m-Triz originates from(i)the stronger adsorption ability of CO_(2)molecule and(ii)the weaker binding energy to form the COOH*intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst,which boosts the conversion of CO_(2)to CO.This research provides a facile way to regulate electrocatalysts for efficient CO_(2)reduction by introducing functionalized molecules.
基金Project supported by the State Key Laboratory of Geohazard Prevention and Geoenvironment Protection(SKLGP2020Z003)。
文摘A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+).Characterization of the materials was carried out using techniques such as X-ray diffraction(XRD),Fourier transform infrared(FTIR),scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS),thermogravimetric analysis(TGA)and Brunauer-Emmett-Teller(BET).The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and mo rphology of MIL-101(Cr).Adsorption experiments were conducted to explore parameters including equilibrium pH,initial Eu3+concentration,and duration,with comprehensive analyses of adsorption kinetics,isotherms,and mechanisms.Findings reveal that Poly(IL1-AA)@MIL-101(Cr),Poly(IL3-AA)@MIL-101(Cr),and Poly(IL5-AA)@MIL-101(Cr)achieve adsorption equilibrium for Eu3+at approximately 9 h with an equilibrium pH of 6.2.The adso rption of Eu^(3+)predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model.Moreover,the prepared composite material exhibits superior adsorption selectivity for Eu^(3+)over other metal ions in the mixture(K^(+),Mg^(2+),Ni^(2+),Co^(2+),Zn^(2+),La^(3+),and Nd^(3+)).Even after five adsorption-desorption cycles,the composite material maintains satis factory adsorption performance.
基金financial support of the Scientific Research Funds of Huaqiao University(605-50Y17073),Xiamen,China.
文摘The composite membrane of microcrystalline cellulose(MCC)with polyvinyl alcohol(PVA)was effectively synthesized using ionic liquids(ILs)as the solvent and dimethyl sulfone(DMSO)as the co-solvent through the phase conversion method.The effects of IL structure and the IL/DMSO mass ratio on the solubility of MCC were investigated.The findings indicated that the composite solvent functioned as a non-derivative solvent for MCC dissolution.The inclusion of DMSO decreased the viscosity of ILs and enhanced the rate of MCC dissolution.The solubility of MCC reached 14.5%(mass)when the mass ratio of[Bmim]Cl to DMSO was 1:1.The fabricated MCC membrane exhibited a smooth surface and a dense structure.PVA@MCC demonstrated exceptional mechanical properties and a uniform structure at a mass ratio of 2:1,with an elongation at break of 76%and a tensile strength of 14.6 MPa.The effects of antibacterial agents on the morphology,transmittance,mechanical properties,and antibacterial efficiency of PVA@MCC were investigated.The findings revealed that PVA@MCC fortified with clove oil showcased a flat and smooth surface,devoid of stratification or aggregation,and demonstrated superior mechanical properties compared to its counterparts with chitosan and ZnO additions.The elongation at break of PVA@MCC with clove oil increased to 137.6%,while its tensile strength decreased to 10.4 MPa.PVA@MCC with clove oil exhibited an antibacterial efficiency exceeding 68%against Escherichia coli,Staphylococcus aureus,and Pseudomonas aeruginosa,thereby extending the shelf life of cherry tomatoes by an additional four days at ambient temperature.
基金supported by the National Natural Science Foundation of China(No.52173095)the MOE Key Laboratory of Macromolecular Synthesis and Functionalization,Zhejiang University(No.2023MSF05)。
文摘The recovery of ionic liquids(ILs)has attracted growing attention as an indispensable process in“green”industrial applications.Forward osmosis(FO)has proven to be a sustainable method for concentrating the very dilute aqueous solutions of ILs at ambient temperature,in which semi-permeable membranes play a vital role in determining the recovery efficiency.Herein,we use interfacial polymerization method to prepare thin-film composite membranes consisting of polyamide skin layer and electrospun nanofibrous substrate with tunable water permeability and IL selectivity for osmotic enrichment of imidazolium ILs from their dilute aqueous solutions through FO process.The resulting FO membrane shows a compact polyamide layer with a thickness of 30-200 nm,guranteeing a high selectivity to ILs and water.Meanwhile,the nanofibrous substrate with large and interconnect pores as well as low tortuosity,providing mechanical and permeable support for the composite membranes.IL structure influences the osmotic pressure difference as well as the interactions with polyamide layer of the membrane and thus determines the whole concentration process.First,the alkyl chain growth augments the osmosis pressure difference between the ILs solution and draw solution,resulting in an enhancement in driving force of water osmosis and IL enrichment.Moreover,alkyl length aggravates external concentration polarization caused by the enhanced adsorption of ILs onto the skin layer via electrostatic and alkyl-πinteractions.Meanwhile,such adsorbed ILs further enhance the IL retention but decrease the reverse salt diffusion.Therefore,imidazolium ILs with varied alkyl lengths are ultimately enriched with a 100-fold increase in concentration from their dilute aqueous solutions with high IL/NaCl rejection and low IL loss.Remarkably,the final concentration of IL with longest alkyl length reaches the highest(6.4 mol·L^(-1)).This work provides the insights in respect to material preparation and process amelioration for IL recovery with high scalability at mild conditions.
基金supported by the National Natural Science Foundation of China(Grant No.52206165)。
文摘Flammable ionic liquids exhibit high conductivity and a broad electrochemical window,enabling the generation of combustible gases for combustion via electrochemical decomposition and thermal decomposition.This characteristic holds significant implications in the realm of novel satellite propulsion.Introducing a fraction of the electrical energy into energetic ionic liquid fuels,the thermal decomposition process is facilitated by reducing the apparent activation energy required,and electrical energy can trigger the electrochemical decomposition of ionic liquids,presenting a promising approach to enhance combustion efficiency and energy release.This study applied an external voltage during the thermal decomposition of 1-ethyl-3-methylimidazole nitrate([EMIm]NO_(3)),revealing the effective alteration of the activation energy of[EMIm]NO_(3).The pyrolysis,electrochemical decomposition,and electron assisted enhancement products were identified through Thermogravimetry-Differential scanning calorimetry-Fourier transform infrared-Mass spectrometry(TG-DSC-FTIR-MS)and gas chromatography(GC)analyses,elucidating the degradation mechanism of[EMIm]NO_(3).Furthermore,an external voltage was introduced during the combustion of[EMIm]NO_(3),demonstrating the impact of voltage on the combustion process.
基金Funding from the Natural Science and Engineering Research Council of Canada(RGPIN-2022-03129)China Scholarship Council(202308210183)the University of Toronto is gratefully acknowledged。
文摘Silver still faces significant challenges in the electrochemical reduction of CO_(2)(eCO_(2)RR)to CO under elevated current density with high energy input due to the intensified hydrogen evolution reaction.The doping of 2 mol%Re-oxide into Ag aerogel results in a significant decrease in the onset potential and a twofold increase in the current density compared to a pure Ag aerogel(Ag100),which tackles the issue.The effect is rationalized in terms of positively shifting the d-band center close to the Fermi energy level to change the density of local electronic states.Moreover,upon the adsorption of the ionic liquid(IL,1-Allyl-3-methylimidazolium dicyanamide[AMIM][DCN])onto the surface of Re-oxide doped Ag aerogel(Ag_(98)Re_(2)/IL),the current density increases to 320 mA/cm^(2) at a low of-1.3 V vs.RHE with 96%selectivity for CO formation in an alkaline medium using a flow cell electrolyzer,and maintains the selectivity above92%for up to 17 h using an H-cell electrolyzer.Density Functional Theory revealed that the adsorbed IL forms a highly conductive and hydrophobic layer on the aerogel surface,presumably decreasing the local H+concentration,greatly suppressing the hydrogen evolution reaction while enhancing the eCO_(2)RR pathway and mitigating the mass transport issues typically associated with IL use.This work addressed the key challenges in massively producing CO from eCO_(2)RR,offering a promising strategy for scalable and industrial CO generation.
