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
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
Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon ele...Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon electrocatalyst(M-N-C)is considered an effective alternative to precious metal catalysts.However,its relatively poor performance in acidic environments has always been a problem plaguing its practical application in PEMFCs.This study presents a sequential deposition methodology for constructing a composite catalytic system of Fe-N-C and ionic liquid(IL),which exhibits improved performance at both half-cell and membrane electrode assembly scales.The presence of IL significantly inhibits H_(2)O_(2)production,preferentially promoting the 4e–O_(2)reduction reaction,resulting in improved electrocatalytic activity and stability.Additionally,the enhanced PEMFC performance of IL containing electrodes is a direct result of the improved ionic and reactant accessibility of the pore confined Fe-N-C catalysts where the IL minimizes local resistive transport losses.This study establishes a strategic foundation for the practical utilization of non-precious metal catalysts in PEMFCs and other energy converting technologies.展开更多
Functionally graded materials (FGMs) are innovative materials distinguished by gradual variations in composition and structure, offering exceptional properties for diverse applications. Poly(ionic liquid)s (PILs), mer...Functionally graded materials (FGMs) are innovative materials distinguished by gradual variations in composition and structure, offering exceptional properties for diverse applications. Poly(ionic liquid)s (PILs), merging the characteristics of polymers and ionic liquids, have emerged as viable options for the development of FGMs given their tunable skeleton, ionic conductivity, and compatibility with various functional materials. This review highlights the latest advancements in the design strategies of FGMs based on porous PILs, focusing on single and multi-gradient structures. Furthermore, we also highlight their emerging applications in molecular recognition, sensing, adsorption, separation, and catalysis. By exploring the interplay between porosity, ionic functionality, and gradient architecture, this review offers perspectives on the prospects of PIL-based FGMs for tackling global challenges in energy, environment, and healthcare.展开更多
Dimethyl carbonate(DMC)is an important chemical raw material extensively used in organic synthesis,lithium-ion battery electrolytes,etc.The primary method for industrial synthesis of DMC involves transesterification b...Dimethyl carbonate(DMC)is an important chemical raw material extensively used in organic synthesis,lithium-ion battery electrolytes,etc.The primary method for industrial synthesis of DMC involves transesterification between ethylene carbonate and MeOH but faces issues with difficult catalyst separation and low catalytic activity.Based on the synergistic catalytic activity of cation and anion,this study develops poly(ionic liquid)s of[N_(X)PIL][PHO]and[N_(3)PIL][Y]with varying alkaline sites and alkalinity levels.This is accomplished by constructing functional polymer monomers containing free radical polymerization sites and nitrogencontaining alkaline groups,and by polymerizing them with suitable crosslinking monomers in a specific ratio before exchanging the resulting polymers with different anions.Results show that doping with nitrogen-containing alkaline groups leads to enhanced basic functional sites while appropriate anions provide intensified alkalinity levels.The[N_(3)PIL][PHO]obtained exhibits superior catalytic activity in transesterification synthesis of DMC,with a yield of 91.43%and selectivity of 99.96%at a reaction time of 2 h.The study also investigates the impact of poly(ionic liquid)cationic structure and anion types,as well as their interactions,on catalytic performance.The findings reveal that the catalytic activity of poly(ionic liquid)is restricted by the interactions between cation and anion.Based on these findings,a possible reaction mechanism was proposed,providing theoretical support for the high-efficiency production of DMC.展开更多
In the context of peaking carbon dioxide emissions and carbon neutrality,development of feasible methods for converting CO_(2)into high value-added chemicals stands out as a hot subject.In this study,P[D+COO^(−)][Br^(...In the context of peaking carbon dioxide emissions and carbon neutrality,development of feasible methods for converting CO_(2)into high value-added chemicals stands out as a hot subject.In this study,P[D+COO^(−)][Br^(−)][DBUH^(+)],a series of novel heterogeneous dual-ionic poly(ionic liquid)s(PILs)were synthesized readily from 2-(dimethylamino)ethyl methacrylate(DMAEMA),bromo-substituted aliphatic acids,organic bases and divinylbenzene(DVB).The structures,compositions and morphologies were characterized or determined by nuclear magnetic resonance(NMR),thermal gravimetric analysis(TGA),infrared spectroscopy(IR),scanning electron microscopes(SEM),and Brunauer-Emmett-Teller analysis(BET),etc.Application of the P[D+COO^(−)][Br^(−)][DBUH^(+)]series as catalysts in converting CO_(2)into cyclic carbonates showed that P[D+COO^(−)][Br^(−)][DBUH^(+)]-2/1/0.6was able to catalyze epiclorohydrin-CO_(2)cycloaddition the most efficiently.This afforded chloropropylene carbonate(CPC)in 98.4%yield with≥99%selectivity in 24 hr under solvent-and additive-free conditions at atmospheric pressure.Reusability experiments showed that recycling of the catalyst 6 times only resulted in a slight decline in the catalytic performance.In addition,it could be used for the synthesis of a variety of differently substituted cyclic carbonates in good to excellent yields.Finally,key catalytic active sites were probed,and a reasonable mechanism was proposed accordingly.In summary,this work poses an efficient strategy for heterogenization of dual-ionic PILs and provides amild and environmentally benign approach to the fixation and utilization of carbon dioxide.展开更多
The potential of organic coatings in antifouling applications has been well-documented.Beyond their exceptional antifouling effects,these coatings should also possess good mechanical strength and self-healing capabili...The potential of organic coatings in antifouling applications has been well-documented.Beyond their exceptional antifouling effects,these coatings should also possess good mechanical strength and self-healing capabilities.Herein,a novel vinyl-based ionic liquid[VEMIM^(+)][Cl^(−)](IL)was in situ polymerized and then assembled onto the surface of liquid metal(GLM)nanodroplets to prepare GLM-IL.Subsequently,Ti_(3)C_(2)Tx(MXene)was modified with GLM-IL nanodroplets to obtain GLM-IL/MXene composite,which acts as an efficient photon captor and photothermal converters and can be further composited with PU film(GLM-IL/MXene/PU).Notably,the composite film significantly increases by∼117℃after exposure to 200 mW/cm2 light irradiation.This increase is attributed to the high photothermal conversion efficiency of MXene and the excellent plasma effect of GLM-IL.Compared with pure PU,the GLM-IL/MXene/PU film shows a 50%improvement in tensile strength and above 85.8%healing efficiency with a local temperature increase.Additionally,the as-prepared GLM-IL/MXene/PU film reveals satisfactory antifouling properties,achieving a 99.7%reduction in bacterial presence and an 80.3%reduction in microalgae.This work introduces a novel coating with antifouling and self-healing properties,offering a wide range of applications in the fields of marine antifouling and biomedicine.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 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
Harvesting energy from humid air to generate electricity represents a promising strategy for sustainable power generation.However,achieving high output and long-term stability in moisture-driven power generators(MPGs)...Harvesting energy from humid air to generate electricity represents a promising strategy for sustainable power generation.However,achieving high output and long-term stability in moisture-driven power generators(MPGs)remains a significant challenge.Here,we develop an efficient MPG by incorporating polymerized ionic liquid(PIL)and MXene through in-situ polymerization of cationic long chains within the MXene layers.This structural design enhances the hydrophilicity and ion dynamics,ensuring stable and sustained electrical output.A single MPG device delivers an open-circuit voltage of 0.65 V and a power density of 14.87 μW·cm^(-2),operating continuously for over 36 h.Surface characterization and quantum chemistry calculations elucidate that the mobile anions within the MPG move directionally under moisture gradients,while polymerized cations remain stationary,driving power generation.The MPG exhibits exceptional long-term stability,retaining about 80%of its initial voltage output after 30 days.Moreover,these MPGs demonstrate scalability for practical applications,capable of efficiently charging capacitors and powering LEDs through simple series-parallel configurations.This work offers a promising strategy to simultaneously enhance the performance and operational stability of MPGs,offering a sustainable solution for the direct conversion of low-grade thermal energy from moisture into clean electricity.展开更多
Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials ...Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.展开更多
N-Methyl-N-propylpiperidiniumbis（trifluoromethanesulfonyl）imide （PP13TFSI）, bis（triflu- oromethanesulfonyl）imide lithium salt （LiTFSI）, and poly（vinylidene difluoride-co- hexafluoropropylene） （P（VdF-HFP）...N-Methyl-N-propylpiperidiniumbis（trifluoromethanesulfonyl）imide （PP13TFSI）, bis（triflu- oromethanesulfonyl）imide lithium salt （LiTFSI）, and poly（vinylidene difluoride-co- hexafluoropropylene） （P（VdF-HFP）） were mixed and made into ionic liquid gel polymer electrolytes （ILGPEs） by solution casting. The morphology of ILGPEs was observed by scanning electron microscopy. It was found that the ILGPE had a loosened structure with liquid phase uniformly distributed. The ionic conductivity, lithium ion transference num- bet and electrochemical window were measured by electrochemical impedance spectroscopy, chronoamperometric and linear sweep voltammetry. The ionic conductivity and lithium ion transference number of this ILGPE reached 0.79 mS/cm and 0.71 at room temperature, and the electrochemical window was 0 to 5.1 V vs. Li＋/Li. Battery tests indicated that the ILGPE is stable when being operated in Li/LiFePO4 batteries. The discharge capacity maintained at about 135, 117, and 100 mAh/g at 30, 75, and 150 mA/g rates, respectively. The capacity retentions were almost 100% after 100 cycles without little capacity fading.展开更多
Fhnctionalized ionic liquid samples （bmim-PW12） were synthesized by 1-butyl-3-methyl- imidazolium bromide （bmimBr） and 12-phosphotungstic heteropolyacid （PW12）. The samples were annealed at 100-450 ℃ and were c...Fhnctionalized ionic liquid samples （bmim-PW12） were synthesized by 1-butyl-3-methyl- imidazolium bromide （bmimBr） and 12-phosphotungstic heteropolyacid （PW12）. The samples were annealed at 100-450 ℃ and were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscope, thermal gravity-DTG, brunauer emmett teller, and NHa-temperature programmed desorption. The results showed that the bmim-PW12 samples were crystal and maintained intact Keggin structure. The organic parts of those samples were partly decomposed at a temperature more than 350 ℃. The sample annealed at 400 ℃ exhibited nano-porous structure, strong acidity, and excellent catalytic activity on the esterification of n-butanol with acetic acid. The higher ester yield was obtained when the mass ratio of catalyst over the reactants amount was 5% for bmim-PW12 catalyst annealed at 400 ℃.展开更多
Ionic liquids(ILs)have appeared as the most promising electrolytes for lithium-ion batteries,owing to their unique high ionic conductivity,chemical stability and thermal stability properties.Poly(ionic liquid)s(PILs)w...Ionic liquids(ILs)have appeared as the most promising electrolytes for lithium-ion batteries,owing to their unique high ionic conductivity,chemical stability and thermal stability properties.Poly(ionic liquid)s(PILs)with both IL-like characteristic and polymer structure are emerging as an alternative of traditional electrolyte.In this review,recent progresses on the applications of IL/PIL-based semi-solid state electrolytes,including gel electrolytes,ionic plastic crystal electrolytes,hybrid electrolytes and single-ion conducting electrolytes for lithium-ion batteries are discussed.展开更多
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.
基金国家自然科学基金(22202124,22208376)山西省科技创新团队专项资金(202304051001023)+3 种基金山西省重点研发计划(202302060301009)山西省国家留学基金委(2023-008,2023-009)山东省自然科学基金(ZR2023LFG005)青岛新能源山东实验室开放项目(QNESL OP 202303).
文摘Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon electrocatalyst(M-N-C)is considered an effective alternative to precious metal catalysts.However,its relatively poor performance in acidic environments has always been a problem plaguing its practical application in PEMFCs.This study presents a sequential deposition methodology for constructing a composite catalytic system of Fe-N-C and ionic liquid(IL),which exhibits improved performance at both half-cell and membrane electrode assembly scales.The presence of IL significantly inhibits H_(2)O_(2)production,preferentially promoting the 4e–O_(2)reduction reaction,resulting in improved electrocatalytic activity and stability.Additionally,the enhanced PEMFC performance of IL containing electrodes is a direct result of the improved ionic and reactant accessibility of the pore confined Fe-N-C catalysts where the IL minimizes local resistive transport losses.This study establishes a strategic foundation for the practical utilization of non-precious metal catalysts in PEMFCs and other energy converting technologies.
基金support provided by National Natural Science Foundation of China(22471018,22071008,22208018)support provided by the Shenzhen Science and Technology Program(JCYJ20220818100012025).
文摘Functionally graded materials (FGMs) are innovative materials distinguished by gradual variations in composition and structure, offering exceptional properties for diverse applications. Poly(ionic liquid)s (PILs), merging the characteristics of polymers and ionic liquids, have emerged as viable options for the development of FGMs given their tunable skeleton, ionic conductivity, and compatibility with various functional materials. This review highlights the latest advancements in the design strategies of FGMs based on porous PILs, focusing on single and multi-gradient structures. Furthermore, we also highlight their emerging applications in molecular recognition, sensing, adsorption, separation, and catalysis. By exploring the interplay between porosity, ionic functionality, and gradient architecture, this review offers perspectives on the prospects of PIL-based FGMs for tackling global challenges in energy, environment, and healthcare.
基金supported by the National Natural Science Foundation of China(Grant No.22278077,22408209 and 22108040)National Key Research and Development Program of China(Grant No.2022YFB4101800)+2 种基金Key Program of Qingyuan Innovation Laboratory(Grant No.00221004)Research Program of Qingyuan Innovation Laboratory(Grant No.00523006)Natural Science Foundation of Fujian Province(Grant No.2022J02019,2024J011550).
文摘Dimethyl carbonate(DMC)is an important chemical raw material extensively used in organic synthesis,lithium-ion battery electrolytes,etc.The primary method for industrial synthesis of DMC involves transesterification between ethylene carbonate and MeOH but faces issues with difficult catalyst separation and low catalytic activity.Based on the synergistic catalytic activity of cation and anion,this study develops poly(ionic liquid)s of[N_(X)PIL][PHO]and[N_(3)PIL][Y]with varying alkaline sites and alkalinity levels.This is accomplished by constructing functional polymer monomers containing free radical polymerization sites and nitrogencontaining alkaline groups,and by polymerizing them with suitable crosslinking monomers in a specific ratio before exchanging the resulting polymers with different anions.Results show that doping with nitrogen-containing alkaline groups leads to enhanced basic functional sites while appropriate anions provide intensified alkalinity levels.The[N_(3)PIL][PHO]obtained exhibits superior catalytic activity in transesterification synthesis of DMC,with a yield of 91.43%and selectivity of 99.96%at a reaction time of 2 h.The study also investigates the impact of poly(ionic liquid)cationic structure and anion types,as well as their interactions,on catalytic performance.The findings reveal that the catalytic activity of poly(ionic liquid)is restricted by the interactions between cation and anion.Based on these findings,a possible reaction mechanism was proposed,providing theoretical support for the high-efficiency production of DMC.
基金supported by the Applied Basic Research Foundation of Guangdong Province(No.2019A1515110551)the Science Foundation for Distinguished Scholars of Dongguan University of Technology(No.196100041051).
文摘In the context of peaking carbon dioxide emissions and carbon neutrality,development of feasible methods for converting CO_(2)into high value-added chemicals stands out as a hot subject.In this study,P[D+COO^(−)][Br^(−)][DBUH^(+)],a series of novel heterogeneous dual-ionic poly(ionic liquid)s(PILs)were synthesized readily from 2-(dimethylamino)ethyl methacrylate(DMAEMA),bromo-substituted aliphatic acids,organic bases and divinylbenzene(DVB).The structures,compositions and morphologies were characterized or determined by nuclear magnetic resonance(NMR),thermal gravimetric analysis(TGA),infrared spectroscopy(IR),scanning electron microscopes(SEM),and Brunauer-Emmett-Teller analysis(BET),etc.Application of the P[D+COO^(−)][Br^(−)][DBUH^(+)]series as catalysts in converting CO_(2)into cyclic carbonates showed that P[D+COO^(−)][Br^(−)][DBUH^(+)]-2/1/0.6was able to catalyze epiclorohydrin-CO_(2)cycloaddition the most efficiently.This afforded chloropropylene carbonate(CPC)in 98.4%yield with≥99%selectivity in 24 hr under solvent-and additive-free conditions at atmospheric pressure.Reusability experiments showed that recycling of the catalyst 6 times only resulted in a slight decline in the catalytic performance.In addition,it could be used for the synthesis of a variety of differently substituted cyclic carbonates in good to excellent yields.Finally,key catalytic active sites were probed,and a reasonable mechanism was proposed accordingly.In summary,this work poses an efficient strategy for heterogenization of dual-ionic PILs and provides amild and environmentally benign approach to the fixation and utilization of carbon dioxide.
基金financially supported by the National Natural Science Foundation of China(No.U21A2046)the Western Light Project of CAS(No.xbzg-zdsys-202118)+1 种基金the Shaanxi Provincial Science and Technology Innovation Team(No.2024RS-CXTD-63)the Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(No.2023-TS-03).
文摘The potential of organic coatings in antifouling applications has been well-documented.Beyond their exceptional antifouling effects,these coatings should also possess good mechanical strength and self-healing capabilities.Herein,a novel vinyl-based ionic liquid[VEMIM^(+)][Cl^(−)](IL)was in situ polymerized and then assembled onto the surface of liquid metal(GLM)nanodroplets to prepare GLM-IL.Subsequently,Ti_(3)C_(2)Tx(MXene)was modified with GLM-IL nanodroplets to obtain GLM-IL/MXene composite,which acts as an efficient photon captor and photothermal converters and can be further composited with PU film(GLM-IL/MXene/PU).Notably,the composite film significantly increases by∼117℃after exposure to 200 mW/cm2 light irradiation.This increase is attributed to the high photothermal conversion efficiency of MXene and the excellent plasma effect of GLM-IL.Compared with pure PU,the GLM-IL/MXene/PU film shows a 50%improvement in tensile strength and above 85.8%healing efficiency with a local temperature increase.Additionally,the as-prepared GLM-IL/MXene/PU film reveals satisfactory antifouling properties,achieving a 99.7%reduction in bacterial presence and an 80.3%reduction in microalgae.This work introduces a novel coating with antifouling and self-healing properties,offering a wide range of applications in the fields of marine antifouling and biomedicine.
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the National Natural Science Foundation of China(22278401 and 92163209)the ANSO Collaborative Research Program(ANSO-CR-KP-2022-12)+2 种基金Beijing Natural Science Foundation(2252011 and JQ22004)Beijing Nova Program(20230484478)for financial supportsupported by Public Computing Cloud,Renmin University of China.
文摘Harvesting energy from humid air to generate electricity represents a promising strategy for sustainable power generation.However,achieving high output and long-term stability in moisture-driven power generators(MPGs)remains a significant challenge.Here,we develop an efficient MPG by incorporating polymerized ionic liquid(PIL)and MXene through in-situ polymerization of cationic long chains within the MXene layers.This structural design enhances the hydrophilicity and ion dynamics,ensuring stable and sustained electrical output.A single MPG device delivers an open-circuit voltage of 0.65 V and a power density of 14.87 μW·cm^(-2),operating continuously for over 36 h.Surface characterization and quantum chemistry calculations elucidate that the mobile anions within the MPG move directionally under moisture gradients,while polymerized cations remain stationary,driving power generation.The MPG exhibits exceptional long-term stability,retaining about 80%of its initial voltage output after 30 days.Moreover,these MPGs demonstrate scalability for practical applications,capable of efficiently charging capacitors and powering LEDs through simple series-parallel configurations.This work offers a promising strategy to simultaneously enhance the performance and operational stability of MPGs,offering a sustainable solution for the direct conversion of low-grade thermal energy from moisture into clean electricity.
基金financially supported by the National Key R&D Program of China(Grant No.2022YFE0207300)National Natural Science Foundation of China(Grant Nos.22179142 and 22075314)+1 种基金Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2024ZB051 and 2023ZB836)the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO).
文摘Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.
文摘N-Methyl-N-propylpiperidiniumbis（trifluoromethanesulfonyl）imide （PP13TFSI）, bis（triflu- oromethanesulfonyl）imide lithium salt （LiTFSI）, and poly（vinylidene difluoride-co- hexafluoropropylene） （P（VdF-HFP）） were mixed and made into ionic liquid gel polymer electrolytes （ILGPEs） by solution casting. The morphology of ILGPEs was observed by scanning electron microscopy. It was found that the ILGPE had a loosened structure with liquid phase uniformly distributed. The ionic conductivity, lithium ion transference num- bet and electrochemical window were measured by electrochemical impedance spectroscopy, chronoamperometric and linear sweep voltammetry. The ionic conductivity and lithium ion transference number of this ILGPE reached 0.79 mS/cm and 0.71 at room temperature, and the electrochemical window was 0 to 5.1 V vs. Li＋/Li. Battery tests indicated that the ILGPE is stable when being operated in Li/LiFePO4 batteries. The discharge capacity maintained at about 135, 117, and 100 mAh/g at 30, 75, and 150 mA/g rates, respectively. The capacity retentions were almost 100% after 100 cycles without little capacity fading.
文摘Fhnctionalized ionic liquid samples （bmim-PW12） were synthesized by 1-butyl-3-methyl- imidazolium bromide （bmimBr） and 12-phosphotungstic heteropolyacid （PW12）. The samples were annealed at 100-450 ℃ and were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscope, thermal gravity-DTG, brunauer emmett teller, and NHa-temperature programmed desorption. The results showed that the bmim-PW12 samples were crystal and maintained intact Keggin structure. The organic parts of those samples were partly decomposed at a temperature more than 350 ℃. The sample annealed at 400 ℃ exhibited nano-porous structure, strong acidity, and excellent catalytic activity on the esterification of n-butanol with acetic acid. The higher ester yield was obtained when the mass ratio of catalyst over the reactants amount was 5% for bmim-PW12 catalyst annealed at 400 ℃.
基金supported by the National Science Fund for Distinguished Young Scholars(No.21425417)the National Natural Science Foundation of China(Nos.21835005 and U1862109)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Ionic liquids(ILs)have appeared as the most promising electrolytes for lithium-ion batteries,owing to their unique high ionic conductivity,chemical stability and thermal stability properties.Poly(ionic liquid)s(PILs)with both IL-like characteristic and polymer structure are emerging as an alternative of traditional electrolyte.In this review,recent progresses on the applications of IL/PIL-based semi-solid state electrolytes,including gel electrolytes,ionic plastic crystal electrolytes,hybrid electrolytes and single-ion conducting electrolytes for lithium-ion batteries are discussed.
