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
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 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
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
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
Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter IL...Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter ILET restricts its use in space missions.To optimize the performance of ILETs and make them suitable for a wider range of space missions,we designed a Circular-emitter ILET(CILET)to convert a one-dimensional(point)emission into a twodimensional(line)emission.The CILET can self-organize multiple Taylor cones simultaneously.The cones were photographed and the axial emission currents were measured under different voltage and pressure difference conditions with a CILET experimental system.The emission can be divided into two stable states and one unstable state based on the flow and current characteristics.The current in Stable state Ⅰ increases non-linearly with the voltage,while that in Stable state Ⅱ is nearly linear with respect to the voltage.The number of cones increases with the voltage in stable states,while the cones become short and crowded under high-voltage conditions.The variation law of the number of cones can be explained with the self-organization theory.The variation in the current exhibits a good correlation with the number of cones.This study demonstrates the feasibility of circular emitters and experimentally indicates that the emission current is improved by approximately two orders of magnitude compared to that of a single capillary.展开更多
Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast pho...Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast photogenerated electron-hole recombination.To tackle these issues,herein,we propose a new strategy to modify Cd_(x) Zn_(1-x) S nanoreactors by the simultaneous utilization of ionic-liquid-assisted morphology engineering and MXene-incorporating method.That is,we designed and synthesized a novel hierarchi-cal Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction composite through the in-situ deposition of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets on unique IL-modified Ti_(3) C_(2) MXenes by a one-pot solvothermal method for efficiently PHE.The unique construction strategy tailors the thickness of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets and prevents them from stacking and agglomeration,and especially,optimizes their charge transfer pathways during the photocatalytic process.Compared with pristine Cd_(0.8) Zn_(0.2) S nanosheets,Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) has abun-dant photogenerated electrons available on the Ti_(3) C_(2) surface for proton reduction reaction,owing to the absence of deep-trapped electrons,suppression of electron-hole recombination in Cd_(0.8) Zn_(0.2) S and high-efficiency charge separation at the Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction interface.Moreover,the hy-drophilicity,electrical conductivity,visible-light absorption capacity,and surficial hydrogen desorption of Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) heterostructure are significantly improved.As a result,the heterostructure exhibits out-standing photocatalytic stability and super high apparent quantum efficiency,being rendered as one of the best noble-metal-free Cd-Zn-S-based photocatalysts.This work illustrates the mechanisms of mor-phology control and heterojunction construction in controlling the catalytic behavior of photocatalysts and highlights the great potential of the IL-assisted route in the synthesis of high-performance MXene-based heterostructures for photocatalytic hydrogen evolution.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
We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisti...We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.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 development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled elec...The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.展开更多
Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.展开更多
The potential toxicity of ionic liquids(ILs)affects their applications;how to control the toxicity is one of the key issues in their applications.To understand its toxicity structure relationship and promote its green...The potential toxicity of ionic liquids(ILs)affects their applications;how to control the toxicity is one of the key issues in their applications.To understand its toxicity structure relationship and promote its greener application,six different machine learning algorithms,including Bagging,Adaptive Boosting(AdaBoost),Gradient Boosting(GBoost),Stacking,Voting and Categorical Boosting(CatBoost),are established to model the toxicity of ILs on four distinct datasets including Leukemia rat cell line IPC-81(IPC-81),Acetylcholinesterase(AChE),Escherichia coli(E.coli)and Vibrio fischeri.Molecular descriptors obtained from the simplified molecular input line entry system(SMILES)are used to characterize ILs.All models are assessed by the mean square error(MSE),root mean square error(RMSE),mean absolute error(MAE)and correlation coefficient(R^(2)).Additionally,an interpretation model based on SHapley Additive exPlanations(SHAP)is built to determine the positive and negative effects of each molecular feature on toxicity.With additional parameters and complexity,the Catboost model outperforms the other models,making it a more reliable model for ILs'toxicity prediction.The results of the model's interpretation indicate that the most significant positive features,SMR_VSA5,PEOE_VSA8,Kappa2,PEOE_VSA6,SMR_VSA5,PEOE_VSA6 and EState_VSA1,can increase the toxicity of ILs as their levels rise,while the most significant negative features,VSA_EState7,EState_VSA8,PEOE_VSA9 and FpDensityMorgan1,can decrease the toxicity as their levels rise.Also,an IL's toxicity will grow as its average molecular weight and number of pyridine rings increase,whereas its toxicity will decrease as its hydrogen bond acceptors increase.This finding offers a theoretical foundation for rapid screening and synthesis of environmentally-benign ILs.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
Oral ulcers may greatly diminish patient life quality and potentially result in malignant transformations.Using gels or films as pseudomembrane barriers is an effective method for promoting ulcer healing.However,these...Oral ulcers may greatly diminish patient life quality and potentially result in malignant transformations.Using gels or films as pseudomembrane barriers is an effective method for promoting ulcer healing.However,these pseudomembranes face challenges such as saliva flushing,dynamic changes,and the presence of abundant microorganisms in the complex oral environment.Herein,we developed an injectable,photoinduction,in situ-enhanceable oral ulcer repair hydrogel(named as GIL2)by incorporating dynamic phenylboronic acid ester bonds and imidazole ions into a methacrylated gelatin matrix.GIL2 exhibited rapid gelation(3 s),low swelling properties(1.07 g/g),robust tensile strength(56.83 kPa)and high adhesive strength(63.38 kPa),allowing it to adhere effectively to the ulcer surface.Moreover,the GIL2 demonstrated intrinsic antibacterial and antioxidant qualities.Within a diabetic rat model for oral ulcers,GIL2 effectively eased oxidative stress and decreased the inflammation present in ulcerated wounds,thereby greatly hastening the healing process of these ulcers.Together,GIL2 hydrogel demonstrates remarkable adaptability within the oral milieu,revitalizing clinical strategy advancements for treating bacterialinfected oral ulcers.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
An ionic liquid assisted hydrogel modified silica was synthesized using a one-pot polymerization and physical coating technique and subsequently applied to mixed-mode liquid chromatography.Analytical techniques,includ...An ionic liquid assisted hydrogel modified silica was synthesized using a one-pot polymerization and physical coating technique and subsequently applied to mixed-mode liquid chromatography.Analytical techniques,including Fourier transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),and elemental analysis,etc.,confirmed the successful prepared of this innovative stationary phase.The unique combination of amide,long alkyl chain,and imidazole ring in the hydrogel coating enables the stationary phase to function effectively in hydrophilic/reversed-phase/ion exchange liquid chromatography.Notably,the stationary phase exhibited superior separation performance owing to the synergistic effect of the ionic liquid and hydrogel.This was particularly evident when analyzing various analytes such as organic acids,nucleosides/bases,polycyclic aromatic hydrocarbons(PAHs)and anions.Furthermore,under our operating conditions,an excellent column efficiency of 53,642.9 plates/m was achieved for theobromine.In summary,we have proposed a straightforward strategy to enhance the separation performance of hydrogel coatings in liquid chromatography,thereby broadening the potential applications of hydrogels in the field of separation.展开更多
The effects of the structure and concentration of impurities on the alkylation of naphthalene with 1-octene catalyzed by chloroaluminate ionic liquid(IL)were investigated.The presence of impurities containing oxygen a...The effects of the structure and concentration of impurities on the alkylation of naphthalene with 1-octene catalyzed by chloroaluminate ionic liquid(IL)were investigated.The presence of impurities containing oxygen and nitrogen led to a decrease in the catalytic performance of chloroaluminate IL.As the water concentration increased to 65 mg·g^(-1),the total selectivity of multi-octylnaphthalene gradually decreased to 42.33%,and the average friction coefficient of the multi-octylnaphthalene base oil gradually increased to 0.201.When the concentration of impurities increased to a critical value,the chloroaluminate IL began to deactivate,leading to a decrease in naphthalene conversion.The critical concentrations for ethanolamine,water,methanol,ether,and diisopentyl sulfide were 33 mg·g^(-1),65 mg·g^(-1),67mg·g^(-1),87 mg·g^(-1),and 123 mg·g^(-1),respectively.Impurities with higher basicity resulted in an earlier onset of chloroaluminate IL deactivation.The changes of Lewis and Brønsted acids in chloroaluminate IL under the influence of impurities were investigated using in situ IR and 27Al NMR spectroscopy.2,6-dimethylpyridine as an indicator could detect the changes of Brønsted acid in chloroaluminate IL better,but the changes of Lewis acid were not obvious because of the overlap between the characteristic peaks.2,6-dichloropyridine as an indicator could exclusively detect the changes of Lewis acid in chloroaluminate IL.With the increase inwater concentration,the Lewis acid in chloroaluminate IL was continuously consumed and converted into Brønsted acid,and the Lewis acid gradually decreased,while the Brønsted acid showed a change of increasing first and then decreasing.展开更多
Due to insufficient energy density,supercapacitors(SCs)with preeminent-power and long cycle stability cannot be implemented in some practical applications.Exploring hybrid materials with redox activity to emerge high ...Due to insufficient energy density,supercapacitors(SCs)with preeminent-power and long cycle stability cannot be implemented in some practical applications.Exploring hybrid materials with redox activity to emerge high specific capacitance in ionic liquid(IL)electrolytes can solve this problem.Herein,we report a redox-organic molecule 2,6-diaminoanthraquinone(DAAQ)modified MXene(Ti3C2Tx)/Graphene(DAAQ-M/G)composite material.With the assist of graphene oxide(GO),MXene and graphene fabricate a three-dimensional(3D)interconnected structure as a conductive framework,which inhibits self-stacking of MXene monolayers and ensures high electronic conductivity.Meanwhile,DAAQ is loaded onto the M/G framework through covalent/non-covalent functionalization.The DAAQ as a spacer effectively enlarges the interlayer spacing of MXene nanosheets,and meanwhile produces reversible redox reactions during charge/discharge processes to provide additional Faradaic contribution to capacity.Therefore,the specific capacitance(capacity)of the DAAQ-M/G as the negative electrode material reaches to 226 F g^(-1)(306 C g^(-1))at 1 A g^(-1)in 1-ethyl-3-methylimidazolium tetrafluoroborate(EmimBF4)electrolyte.Furthermore,an asymmetric supercapacitor(ASC)is assembled using DAAQ-M/G as the negative electrode and self-prepared organic molecule hydroquinone modified reduced graphene oxide(HQ-RGO)material as the positive electrode,with a high energy density of 43 Wh kg^(-1)at high power density of 1669 Wkg^(-1).The ASC can maintain 80%of initial specific capacitance after 9000 cycles.This research can provide better support to develop advanced organic molecules-modified MXene composite materials for ionic liquid-based SCs.展开更多
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 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financially supported by the National Key R&D Program of China(Grant No.2022YFE0207300)National Natural Science Foundation of China(Grant Nos.22179142 and 22075314)+1 种基金Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2024ZB051 and 2023ZB836)the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO).
文摘Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.
基金co-supported by the National Key R&D Program of China(No.2020YFC2201001)the Shenzhen Science and Technology Program,China(No.20210623091808026)。
文摘Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter ILET restricts its use in space missions.To optimize the performance of ILETs and make them suitable for a wider range of space missions,we designed a Circular-emitter ILET(CILET)to convert a one-dimensional(point)emission into a twodimensional(line)emission.The CILET can self-organize multiple Taylor cones simultaneously.The cones were photographed and the axial emission currents were measured under different voltage and pressure difference conditions with a CILET experimental system.The emission can be divided into two stable states and one unstable state based on the flow and current characteristics.The current in Stable state Ⅰ increases non-linearly with the voltage,while that in Stable state Ⅱ is nearly linear with respect to the voltage.The number of cones increases with the voltage in stable states,while the cones become short and crowded under high-voltage conditions.The variation law of the number of cones can be explained with the self-organization theory.The variation in the current exhibits a good correlation with the number of cones.This study demonstrates the feasibility of circular emitters and experimentally indicates that the emission current is improved by approximately two orders of magnitude compared to that of a single capillary.
基金financial supports pro-vided by the National Natural Science Foundation of China(No.21905279)the Natural Science Foundation of Fujian Province(No.2020J05086).
文摘Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast photogenerated electron-hole recombination.To tackle these issues,herein,we propose a new strategy to modify Cd_(x) Zn_(1-x) S nanoreactors by the simultaneous utilization of ionic-liquid-assisted morphology engineering and MXene-incorporating method.That is,we designed and synthesized a novel hierarchi-cal Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction composite through the in-situ deposition of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets on unique IL-modified Ti_(3) C_(2) MXenes by a one-pot solvothermal method for efficiently PHE.The unique construction strategy tailors the thickness of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets and prevents them from stacking and agglomeration,and especially,optimizes their charge transfer pathways during the photocatalytic process.Compared with pristine Cd_(0.8) Zn_(0.2) S nanosheets,Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) has abun-dant photogenerated electrons available on the Ti_(3) C_(2) surface for proton reduction reaction,owing to the absence of deep-trapped electrons,suppression of electron-hole recombination in Cd_(0.8) Zn_(0.2) S and high-efficiency charge separation at the Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction interface.Moreover,the hy-drophilicity,electrical conductivity,visible-light absorption capacity,and surficial hydrogen desorption of Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) heterostructure are significantly improved.As a result,the heterostructure exhibits out-standing photocatalytic stability and super high apparent quantum efficiency,being rendered as one of the best noble-metal-free Cd-Zn-S-based photocatalysts.This work illustrates the mechanisms of mor-phology control and heterojunction construction in controlling the catalytic behavior of photocatalysts and highlights the great potential of the IL-assisted route in the synthesis of high-performance MXene-based heterostructures for photocatalytic hydrogen evolution.
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We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.
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supported by the National Natural Science Foundation of China(22209040,22202063).
文摘The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
基金funded by Research Platforms and Projects for Higher Education Institutions of Department of Education of Guangdong Province in 2024(2024KTSCX256)2023 Guangdong Province Higher Vocational Education Teaching Quality and Teaching Reform Project(2023JG080).
文摘The potential toxicity of ionic liquids(ILs)affects their applications;how to control the toxicity is one of the key issues in their applications.To understand its toxicity structure relationship and promote its greener application,six different machine learning algorithms,including Bagging,Adaptive Boosting(AdaBoost),Gradient Boosting(GBoost),Stacking,Voting and Categorical Boosting(CatBoost),are established to model the toxicity of ILs on four distinct datasets including Leukemia rat cell line IPC-81(IPC-81),Acetylcholinesterase(AChE),Escherichia coli(E.coli)and Vibrio fischeri.Molecular descriptors obtained from the simplified molecular input line entry system(SMILES)are used to characterize ILs.All models are assessed by the mean square error(MSE),root mean square error(RMSE),mean absolute error(MAE)and correlation coefficient(R^(2)).Additionally,an interpretation model based on SHapley Additive exPlanations(SHAP)is built to determine the positive and negative effects of each molecular feature on toxicity.With additional parameters and complexity,the Catboost model outperforms the other models,making it a more reliable model for ILs'toxicity prediction.The results of the model's interpretation indicate that the most significant positive features,SMR_VSA5,PEOE_VSA8,Kappa2,PEOE_VSA6,SMR_VSA5,PEOE_VSA6 and EState_VSA1,can increase the toxicity of ILs as their levels rise,while the most significant negative features,VSA_EState7,EState_VSA8,PEOE_VSA9 and FpDensityMorgan1,can decrease the toxicity as their levels rise.Also,an IL's toxicity will grow as its average molecular weight and number of pyridine rings increase,whereas its toxicity will decrease as its hydrogen bond acceptors increase.This finding offers a theoretical foundation for rapid screening and synthesis of environmentally-benign ILs.
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funding from the National Natural Science Foundation of China(Nos.82071170 and 82371016)the Zhejiang Provincial Science and Technology Project for Public Welfare(No.LGF21H140004).
文摘Oral ulcers may greatly diminish patient life quality and potentially result in malignant transformations.Using gels or films as pseudomembrane barriers is an effective method for promoting ulcer healing.However,these pseudomembranes face challenges such as saliva flushing,dynamic changes,and the presence of abundant microorganisms in the complex oral environment.Herein,we developed an injectable,photoinduction,in situ-enhanceable oral ulcer repair hydrogel(named as GIL2)by incorporating dynamic phenylboronic acid ester bonds and imidazole ions into a methacrylated gelatin matrix.GIL2 exhibited rapid gelation(3 s),low swelling properties(1.07 g/g),robust tensile strength(56.83 kPa)and high adhesive strength(63.38 kPa),allowing it to adhere effectively to the ulcer surface.Moreover,the GIL2 demonstrated intrinsic antibacterial and antioxidant qualities.Within a diabetic rat model for oral ulcers,GIL2 effectively eased oxidative stress and decreased the inflammation present in ulcerated wounds,thereby greatly hastening the healing process of these ulcers.Together,GIL2 hydrogel demonstrates remarkable adaptability within the oral milieu,revitalizing clinical strategy advancements for treating bacterialinfected oral ulcers.
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Innovation Groups of Basic Research in Gansu Province(No.23JRRA570)。
文摘An ionic liquid assisted hydrogel modified silica was synthesized using a one-pot polymerization and physical coating technique and subsequently applied to mixed-mode liquid chromatography.Analytical techniques,including Fourier transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),and elemental analysis,etc.,confirmed the successful prepared of this innovative stationary phase.The unique combination of amide,long alkyl chain,and imidazole ring in the hydrogel coating enables the stationary phase to function effectively in hydrophilic/reversed-phase/ion exchange liquid chromatography.Notably,the stationary phase exhibited superior separation performance owing to the synergistic effect of the ionic liquid and hydrogel.This was particularly evident when analyzing various analytes such as organic acids,nucleosides/bases,polycyclic aromatic hydrocarbons(PAHs)and anions.Furthermore,under our operating conditions,an excellent column efficiency of 53,642.9 plates/m was achieved for theobromine.In summary,we have proposed a straightforward strategy to enhance the separation performance of hydrogel coatings in liquid chromatography,thereby broadening the potential applications of hydrogels in the field of separation.
基金financial support of the Scientific Research Funds of Huaqiao University (605-50Y17073)
文摘The effects of the structure and concentration of impurities on the alkylation of naphthalene with 1-octene catalyzed by chloroaluminate ionic liquid(IL)were investigated.The presence of impurities containing oxygen and nitrogen led to a decrease in the catalytic performance of chloroaluminate IL.As the water concentration increased to 65 mg·g^(-1),the total selectivity of multi-octylnaphthalene gradually decreased to 42.33%,and the average friction coefficient of the multi-octylnaphthalene base oil gradually increased to 0.201.When the concentration of impurities increased to a critical value,the chloroaluminate IL began to deactivate,leading to a decrease in naphthalene conversion.The critical concentrations for ethanolamine,water,methanol,ether,and diisopentyl sulfide were 33 mg·g^(-1),65 mg·g^(-1),67mg·g^(-1),87 mg·g^(-1),and 123 mg·g^(-1),respectively.Impurities with higher basicity resulted in an earlier onset of chloroaluminate IL deactivation.The changes of Lewis and Brønsted acids in chloroaluminate IL under the influence of impurities were investigated using in situ IR and 27Al NMR spectroscopy.2,6-dimethylpyridine as an indicator could detect the changes of Brønsted acid in chloroaluminate IL better,but the changes of Lewis acid were not obvious because of the overlap between the characteristic peaks.2,6-dichloropyridine as an indicator could exclusively detect the changes of Lewis acid in chloroaluminate IL.With the increase inwater concentration,the Lewis acid in chloroaluminate IL was continuously consumed and converted into Brønsted acid,and the Lewis acid gradually decreased,while the Brønsted acid showed a change of increasing first and then decreasing.
基金supported by the National Natural Science Foundation of China(Nos.22173028,21873026).
文摘Due to insufficient energy density,supercapacitors(SCs)with preeminent-power and long cycle stability cannot be implemented in some practical applications.Exploring hybrid materials with redox activity to emerge high specific capacitance in ionic liquid(IL)electrolytes can solve this problem.Herein,we report a redox-organic molecule 2,6-diaminoanthraquinone(DAAQ)modified MXene(Ti3C2Tx)/Graphene(DAAQ-M/G)composite material.With the assist of graphene oxide(GO),MXene and graphene fabricate a three-dimensional(3D)interconnected structure as a conductive framework,which inhibits self-stacking of MXene monolayers and ensures high electronic conductivity.Meanwhile,DAAQ is loaded onto the M/G framework through covalent/non-covalent functionalization.The DAAQ as a spacer effectively enlarges the interlayer spacing of MXene nanosheets,and meanwhile produces reversible redox reactions during charge/discharge processes to provide additional Faradaic contribution to capacity.Therefore,the specific capacitance(capacity)of the DAAQ-M/G as the negative electrode material reaches to 226 F g^(-1)(306 C g^(-1))at 1 A g^(-1)in 1-ethyl-3-methylimidazolium tetrafluoroborate(EmimBF4)electrolyte.Furthermore,an asymmetric supercapacitor(ASC)is assembled using DAAQ-M/G as the negative electrode and self-prepared organic molecule hydroquinone modified reduced graphene oxide(HQ-RGO)material as the positive electrode,with a high energy density of 43 Wh kg^(-1)at high power density of 1669 Wkg^(-1).The ASC can maintain 80%of initial specific capacitance after 9000 cycles.This research can provide better support to develop advanced organic molecules-modified MXene composite materials for ionic liquid-based SCs.
