A new type of rubidium ion-imprinted polymer has been synthesized by the surface-imprinting technique using methacrylic acid as the functional monomer,the rubidium ion as the template,methanol as the solvent,and silic...A new type of rubidium ion-imprinted polymer has been synthesized by the surface-imprinting technique using methacrylic acid as the functional monomer,the rubidium ion as the template,methanol as the solvent,and silica as a carrier.Ethylene glycol dimethacrylate and 2,2-azobisisobutyronitrile were used as acrosslinker and an initiator,respectively.In addition,based on the macrocyclic effect of crown ethers,the 18-crown-6 ligand was introduced as a ligand to fix the template ions better.Scanning electron microscopy,zeta-potential analysis,Fourier transform infrared spectroscopy,thermogravimetric analysis,and X-ray photoelectron spectroscopy were performed to characterize the ion-imprinted polymer.The effects of the preparation and adsorption conditions on the adsorption performance of the rubidium ion-imprinted polymer were investigated.The results indicated that the rubidium ion-imprinted polymer has high selectivity and faster kinetics than other adsorbents,with an equilibrium adsorption capacity of 200.19 mg·g^(-1)at 298 K within 25 min.The sorption isotherm was well described by the Freundlich isotherm model,while the adsorption kinetics fitted the pseudo-second-order kinetic model.Consecutive adsorption-desorption experiments showed that the ion-imprinted polymer had good chemical stability and reusability.展开更多
Levulinic acid(LA)is one of the top-12 most promising biomass-based platform chemicals,which has a wide range of applications in a variety of fields.However,separation and purification of LA from aqueous solution or a...Levulinic acid(LA)is one of the top-12 most promising biomass-based platform chemicals,which has a wide range of applications in a variety of fields.However,separation and purification of LA from aqueous solution or actual hydrolysate continues to be a challenge.Among various downstream separation technologies,liquid-liquid extraction is a low-cost,effective,and simple process to separate LA.The key breakthrough lies in the development of extractants with high extraction efficiency,good hydrophobicity,and low cost.In this work,three hydrophobic deep eutectic solvents(DESs)based on tri-n-octylamine(TOA)as hydrogen bond acceptor(HBA)and alcohols(butanol,2-octanol,and menthol)as hydrogen bond donors(HBDs)were developed to extract LA from aqueous solution.The molar ratios of HBD and HBA,extraction temperature,contact time,solution pH,and initial LA concentration,DES/water volume ratios were systematically investigated.Compared with 2-octanol-TOA and menthol-TOA DES,the butanol-TOA DES exhibited the superior extraction performance for LA,with a maximum extraction efficiency of 95.79±1.4%.Moreover,the solution pH had a great impact on the LA extraction efficiency of butanol-TOA(molar ratio=3:1).It is worth noting that the extraction equilibrium time was less than 0.5 h.More importantly,the butanol-TOA(3:1)DES possesses good extraction abilities for low,medium,and high concentrations of LA.展开更多
Ozone(O_(3)) generated by a dielectric barrier discharge(DBD) is widely used in various industrial processes. In this study, NaCl aqueous solution was used as a novel electric power transmission electrode in a DBD rea...Ozone(O_(3)) generated by a dielectric barrier discharge(DBD) is widely used in various industrial processes. In this study, NaCl aqueous solution was used as a novel electric power transmission electrode in a DBD reactor(instead of a traditional metal electrode) for highly efficient ozone generation. The results demonstrated that a high O_(3) yield of 242 g k Wh^(-1) with a concentration of 14.6 g m^(-3)O_(3) was achieved. The power transmission mechanism works because NaCl aqueous solution behaves as a capacitor when an alternating pulse voltage below 8 k Hz is used.Compared with the resistance of the discharge barrier and discharge space, the resistance of NaCl aqueous solution can be ignored, which ensures that O_(3) is generated efficiently. It is expected that O_(3) generation using NaCl aqueous solution as a novel electrode in a DBD reactor could be an alternative technology with good application prospects.展开更多
Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is...Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is proposed by using molecular dynamics simulation,and the relationship between ion-to-ion interaction and salt solubility in a simulated seawater water-salt system is investigated.By analyzing the variation of distance and contact time between ions in an electrolyte solution,from both spatial and temporal perspectives,new parameters were proposed to describe the interaction between ions:interaction distance(ID),and interaction time ratio(ITR).The best correlation between characteristic time ratio and solubility was found for a molar ratio of salt-to-water of 10:100 with a correlation coefficient of 0.96.For the same salt,a positive correlation was found between CTR and the molar ratio of salt and water.For type 1-1,type 2-1,type 1-2,and type 2-2 salts,the correlation coefficients between CTR and solubility were 0.93,0.96,0.92,and 0.98 for a salt-to-water molar ratio of 10:100,respectively.The solubility of multiple salts was predicted by simulations and compared with experimental values,yielding an average relative deviation of 12.4%.The new ion-interaction parameters offer significant advantages in describing strongly correlated and strongly hydrated electrolyte solutions.展开更多
1,5-Pentanediamine(PDA)produced by biological fermentation becomes popular,but the separation of PDA from the broth is a typical difficult problem.In this work,the performance of 200 ionic liquids(ILs),formed by combi...1,5-Pentanediamine(PDA)produced by biological fermentation becomes popular,but the separation of PDA from the broth is a typical difficult problem.In this work,the performance of 200 ionic liquids(ILs),formed by combining 25 cations and 8 anions,in the extraction of PDA from aqueous solution were evaluated using COSMO-RS model.The extraction mechanism was investigated with the help ofσ-profile and interaction energy analyses.Both the cation and anion have impacts on the extraction efficiency,where cation mainly influences the interaction of IL with PDA and anion affects the hydrophobicity of IL.The IL composed of long alkyl-chain in cation and the anion of[PF6]-or[TF2 N]-,which has theσ-profile more likely distributed in the nonpolar region but less distributed in the polar region,is favorable for extraction.The experimental liquid-liquid equilibrium demonstrated the effects of cation and anion on extraction performance,which validated the reliability of COSMO-RS model in IL screening for PDA extraction.The IL[IM-1,8][PF6]could serve as a promising extractant for the downstream separation process of the biological production of PDA.展开更多
Ionic liquids (ILs) have been regarded as the potential novel solvents for improved analytical- and process-scale separation methods.The development of methods for the recovery of ILs from aqueous solutions to escap...Ionic liquids (ILs) have been regarded as the potential novel solvents for improved analytical- and process-scale separation methods.The development of methods for the recovery of ILs from aqueous solutions to escape contamination and recycle samples will ultimately govern the viability of ILs in the future industrial applications. Therefore, in this paper a new method for separation of ILs from their dilute aqueous solutions and simultaneously purification of water was proposed on the basis of the CO2 hydrate formation. For illustration, the dilute aqueous solutions with concentrations of ILs ranging from 2× 10^-3 mol% to 2×10^-1 mol% were concentrated. The results show that the separation efficiency is very impressive and that the new method is applicable to aqueous solutions of both hydrophobic and hydrophilic ILs. Compared to the literature separation method based on the supercritical CO2, the new method is applicable to lower concentrations, and more importantly, its operation condition is mild.展开更多
Coal fly ash(CFA)is composed of minerals containing some oxides in crystalline phase(i.e.,quartz and mullite),as well as unburned carbon as mesoporous material,thus enabling CFA to act as a dual-sites adsorbent with u...Coal fly ash(CFA)is composed of minerals containing some oxides in crystalline phase(i.e.,quartz and mullite),as well as unburned carbon as mesoporous material,thus enabling CFA to act as a dual-sites adsorbent with unique properties.This work focused on the adsorption of Pb(Ⅱ)and Zn(Ⅱ)from binary system,a mixture containing two metal ion solutions present simultaneously,onto NaOH-modified CFA(MCFA).Several adsorption tests were conducted to evaluate the effect of several parameters,including pH and contact times.The experiment results indicated that chemical treatment of CFA with NaOH increased pore volume from 0.021 to 0.223 cm^3·g^(-1).In addition,it could also enhance the availability of functional groups on both minerals and unburned carbon,resulting in almost 100%Pb(Ⅱ)and 97%Zn(Ⅱ)adsorbed.The optimum pH for adsorption system was pH=3 and quasi-equilibrium occurred in 240 minutes.Equilibrium data from the experimental results were analyzed using Modified Extended Langmuir(MEL)and Competitive Adsorption Langmuir-Langmuir(CALL)isotherm models.The analysis results showed that the CALL isotherm model could better describe the Pb(Ⅱ)and Zn(Ⅱ)adsorption process onto MCFA in binary system compared with MEL isotherm model.展开更多
To investigate the degradation of corrosion resistance of Zircaloy-4 in LiOHaqueous solution, SIMS (secondary ion mass spectrometry) analysis was performed to examine theprofiles of Li^+, K^+, and OH^- in oxide layers...To investigate the degradation of corrosion resistance of Zircaloy-4 in LiOHaqueous solution, SIMS (secondary ion mass spectrometry) analysis was performed to examine theprofiles of Li^+, K^+, and OH^- in oxide layers formed in the same concentration (0.1 mol/L) LiOHand KOH solutions. Even though the oxide layers have an equal thickness, the pene-tration depth ofK^+ is shallower than that of Li^+, and the penetration depth of OH^- corroded in KOH solution isalso shal-ower than that corroded in LiOH solution. It shows that the diffusion of OH^- into oxidelayer is accompanied by the corresponding cation. The difference of degradation effect of LiOH andKOH solutions on the corrosion resistance of Zircaloy-4 was discussed.展开更多
Chemical effects in different aqueous solutions induced by plasma with glow discharge electrolysis (GDE) and contact glow discharge electrolysis (CGDE) are described in this paper. The experimental and discharge char...Chemical effects in different aqueous solutions induced by plasma with glow discharge electrolysis (GDE) and contact glow discharge electrolysis (CGDE) are described in this paper. The experimental and discharge characteristics are also reviewed. These are followed by a discussion of their mechanisms of both anodic and cathodic CGDE..展开更多
Degradation of α-naphthol induced by plasma in aqueous solution was investigated in different initial concentration with contact glow discharge electrolysis(CGDE). The results showed that the degradation of α-naphth...Degradation of α-naphthol induced by plasma in aqueous solution was investigated in different initial concentration with contact glow discharge electrolysis(CGDE). The results showed that the degradation of α-naphthol obeyed the first-rate law. Some of predominant products were analyzed by a high performance liquid chromatography (HPLC). A path of α-naphthol disappearance caused by plasma was proposed according to the detected intermediate products.展开更多
Carbonate-bearing fluids widely exist in different geological settings,and play important roles in transporting some elements such as the rare earth elements.They may be trapped as large or small fluid inclusions(with...Carbonate-bearing fluids widely exist in different geological settings,and play important roles in transporting some elements such as the rare earth elements.They may be trapped as large or small fluid inclusions(with the size down to<1μm sometimes),and record critical physical-chemical signals for the formations of their host minerals.Spectroscopic methods like Raman spectroscopy and infrared spectroscopy have been proposed as effective methods to quantify the carbonate concentrations of these fluid inclusions.Although they have some great technical advantages over the conventional microthermometry method,there are still some technical difficulties to overcome before they can be routinely used to solve relevant geological problems.The typical limitations include their interlaboratory difference and poor performance on micro fluid inclusions.This study prepared standard ion-distilled water and K_(2)CO_(3)aqueous solutions at different molarities(from 0.5 to 5.5 mol/L),measured densities,collected Raman and infrared spectra,and explored correlations between the K_(2)CO_(3)molarity and the spectroscopic features at ambient P-T conditions.The result confirms that the Raman O-H stretching mode can be used as an internal standard to determine the carbonate concentrations despite some significant differences among the correlations,established in different laboratories,between the relative Raman intensity of the C-O symmetric stretching mode and that of the O-H stretching mode.It further reveals that the interlaboratory difference can be readily removed by performing one high-quality calibration experiment,provided that later quantifying analyses are conducted using the same Raman spectrometer with the same analytical conditions.Our infrared absorption data were collected from thin fluid films(thickness less than~2μm)formed by pressing the prepared solutions in a Microcompression Cell with two diamond-II plates.The data show that both the O-H stretching mode and the O-H bending mode can be used as internal standards to determine the carbonate concentrations.Since the IR signals of the C-O antisymmetric stretching vibration of the CO32ion,and the O-H stretching and bending vibrations from our thin films are very strong,their relative IR absorbance intensity,if well calibrated,can be used to investigate the micron-sized carbonate-bearing aqueous fluid inclusions.This study establishes the first calibration of this kind,which may have some applications.Additionally,our spectroscopic data suggest that as the K_(2)CO_(3)concentration increases the aqueous solution forms more large water molecule clusters via more intense hydrogen-bonding.This process may significantly alter the physical and chemical behavior of the fluids.展开更多
We compared the photochemical reaction of m-cresol containing ·OH precursors such as H2O2, NO2 and NO3 in aqueous solution with those in ice. The results show that the conversion rate of m-cresol in aqueous solut...We compared the photochemical reaction of m-cresol containing ·OH precursors such as H2O2, NO2 and NO3 in aqueous solution with those in ice. The results show that the conversion rate of m-cresol in aqueous solution was higher than that in ice. H2O2, NO2 and NO3 all accelerated the photoconversion of m-cresol in both aqueous solution and ice. The photochemical reactions of m-cresol obeys the first order kinetics equation. According to the photoproducts identified by GC-MS, we proposed that hydroxylation and nitration reactions occurred in both aqueous solution and ice. Coupling reaction was common in ice, however, in aqueous solution it was found only in UV system. Our results suggest that the photochemical reactions of m-cresol were different in aqueous solution and in ice.展开更多
The objective of this work is to contribute an understanding of the effects of electrons in the plasmas on the mass transfer of plasma species in aqueous solution by means of the numerical simulation based on a one-di...The objective of this work is to contribute an understanding of the effects of electrons in the plasmas on the mass transfer of plasma species in aqueous solution by means of the numerical simulation based on a one-dimensional diffusion-reaction model.The plasma species are divided into two groups,i.e.electrons and the other species,and the mass transfer in the three scenarios has been simulated,including the systematic calculations of the depth distributions of five major reactive species,OH,O3,HO2,O2^-,and H2O2.In the three scenarios,the particles considered to enter into aqueous solution are all the plasma species(the scenario Ⅰ,where the mass transfer of plasma species is a result due to the synergy of the electrons and the other plasma species),the other species(the scenario Ⅱ),and only electrons in plasma species(the scenario Ⅲ),respectively.The detailed analyses on the difference between the depth distributions of each reactive species in these three scenarios show the following conclusions.The electrons play an important role in the mass transfer of plasma species in aqueous solution and the synergy of the electrons and the other plasma species(the electron-species synergy)presents its different effects on the mass transfer.The vast majority of H2O2 are generated from a series of the electronrelated reactions in aqueous solution,which is hardly affected by the electron-species synergy.Compared to the results when only the electrons enter into the liquid region,the electron-species synergy evidently weakens the generation of O2^-,O3,and OH,but promotes to produce HO2.展开更多
Agglomeration-free nanosized ZrO2-HfO2-Y2O3-Sc2O3 composite powders were successfully synthesized by Sol-Gel technique in heated aqueous solution of alcohol, using analytically pure ZrOCl2 · 8H2O, HfOCl2·8H2...Agglomeration-free nanosized ZrO2-HfO2-Y2O3-Sc2O3 composite powders were successfully synthesized by Sol-Gel technique in heated aqueous solution of alcohol, using analytically pure ZrOCl2 · 8H2O, HfOCl2·8H2O, Y(NO3)3·6H2O, and Sc2O3 as raw materials. The effect of synthesis condition on the size and dispersity of the composite powders was investigated by means of XRD, TEM, and TG-DSC techniques. The results showed that well-dispersed predecessor of ZrO2-HfO2-Y2O3-Sc2O3 composite nanopowders could be obtained. The optional condition : PEG6000 as dispersant was 1%, alcohol/H2O ratio was 5/1, metallic ion concentration in whole solution was 0.5 mol·L^-1 and the pH value of the solution was 12. After calcined at 620 ℃, the powder obtained was in uniform cubic structure, and its average particle size was about 13 nm, which was good for producing nanocrystalline solid electrolyte.展开更多
In this work,an air-blast atomizing column was used to study the CO2 capture performance with aqueous MEA(mono-ethanol-amine)and Na OH solutions.The effects of gas flow rate,the liquid to gas ratio(L/G),the CO2 concen...In this work,an air-blast atomizing column was used to study the CO2 capture performance with aqueous MEA(mono-ethanol-amine)and Na OH solutions.The effects of gas flow rate,the liquid to gas ratio(L/G),the CO2 concentration on the CO2 removal efficiency(η)and the volumetric overall mass transfer coefficient(KGav)were investigated.The air-blast atomizing column was also compared with the pressure spray tower on the studies of the CO2 capture performance.For the aqueous MEA and Na OH solutions,the experimental results show that theηdecreases with increasing gas flow rate and CO2 concentration while it increases with increasing L/G.The effects on KGavare more complicated than those forη.When the CO2 concentration is low(3 vol%),KGavincreases with increasing gas flow rate while decreases with increasing L/G.However,when the CO2 concentration is high(9.5 vol%),as the gas flow rate and L/G increases,KGavincreases first and then decreases.The aqueous MEA solution achieves higherηand KGavthan the aqueous Na OH solution.The air-blast atomizing column shows a good performance on CO2 capture.展开更多
The reverse osmosis (RO) separation of aqueous organic solutions, such as alcohols, amines, aldehydes, acids, ketones, and esters etc., by PAA (polyacrylic acid)/PSF (polysulfone) composite membrane has been studied. ...The reverse osmosis (RO) separation of aqueous organic solutions, such as alcohols, amines, aldehydes, acids, ketones, and esters etc., by PAA (polyacrylic acid)/PSF (polysulfone) composite membrane has been studied. It was found that the separation results for aliphatic alcohols, amines and aldehydes are satisfactory, the solute rejection (R-a) and the volume fluxes of solutions (J(V)) for 1000 ppm ethanol, ethylamine and ethyl aldehyde are 66.2%, 61.0%, 84.0% and 0.90 x 10(-6), 0.35 x 10(-6), 0.40 X 10(-6) m(3)/m(2) . s, respectively, at 5.0 MPa and 30 degrees C. R-a increased with increasing molecular weights of alcohols, amines and aldehydes, and the R-a for n-amyl alcohol, n-butylamine and n-butyl aldehyde reached 94.3%, 88.6% and 96.0%, respectively. Satisfactory separation results (R-a > 70%) for ketones, esters, phenols and polyols have been obtained with the PAA/PSF composite membrane. The effect of operating pressure on the properties of reverse osmosis has also been investigated. Analysis of experimental data with Spiegler-Kedem's transport model has been carried out and the membrane constants such as reflection coefficient sigma, solute and hydraulic permeabilities omega and L-p for several organic solutes have been obtained.展开更多
Quaternized cellulose( QC) derivatives were synthesized by reacting cellulose with 3-chloro-2-hydroxypropyl trimethyl ammonium chloride( CHPTAC) in an aqueous solution of Na OH-urea. The chemical structures and physic...Quaternized cellulose( QC) derivatives were synthesized by reacting cellulose with 3-chloro-2-hydroxypropyl trimethyl ammonium chloride( CHPTAC) in an aqueous solution of Na OH-urea. The chemical structures and physical properties of the obtained QC derivatives were characterized using nitrogen content analysis,Fourier transform infrared spectroscopy( FT-IR),~1H-nuclear magnetic resonance(1H-NMR),X-ray diffraction( XRD),and thermal gravity analysis( TGA). The FT-IR and ~1H-NMR results confirmed the successful introduction of cationic quaternary ammonium groups into the main chain of cellulose. A series of QC derivatives with the degree of substitution( DS) values ranging from 0. 33 to 0. 80 were derived by adjusting the molar ratio of CHPTAC to anhydroglucose unit( AGU) of cellulose,concentration of cellulose in the Na OH-urea solution,as well as reaction temperature and time. According to the DS values of the QC derivatives,the optimized synthetic conditions were as follows: 25℃ reaction temperature,3% cellulose in Na OH-urea solution,the molar ratio of etherification agent to glycosidic cellulose of 15∶ 1,and 12 h reaction time. The TGA and XRD results revealed that the crystalline structure was destroyed during etherification,and the thermal stability of the QC derivatives was lower than that of cellulose.展开更多
To solve the environmental pollution and low yield during the sythesis of zeolitic imidazolate frameworks(ZIFs)and their derived materials,a KOH-assisted aqueous strategy is proposed to synthesize cobalt zeolitic imid...To solve the environmental pollution and low yield during the sythesis of zeolitic imidazolate frameworks(ZIFs)and their derived materials,a KOH-assisted aqueous strategy is proposed to synthesize cobalt zeolitic imidazolate framework(ZIF-67)polyhedrons,which are used as precursors to prepare cobalt selenide/carbon composites with different crystal phases(Co_(0.85)Se,CoSe_2).When evaluated as anode material for lithium ion batteries,Co_(0.85)Se/C composites deliver a reversible capacity of 758.7 m A·h·g^(-1)with a capacity retention rate of 90.5%at 1.0 A·g^(-1)after 500 cycles,and the superior rate capability is 620 m A·h·g^(-1)at 2.0 A·g^(-1).The addition of KOH accelerates the production of ZIF-67 crystals by boosting deprotonation of dimethylimidazole,resulting in rapid growth and structures transition from two-dimensional to three-dimensional of ZIF-67 in aqueous solution,which greatly promotes the application of MOFs in the field of energy storage and conversion.展开更多
How to determine accurately the association states of solutes in aqueous systems is of fundamental importance in a variety of chemical, physical, and biological processes, We apply four widely used criteria to analyze...How to determine accurately the association states of solutes in aqueous systems is of fundamental importance in a variety of chemical, physical, and biological processes, We apply four widely used criteria to analyze the dynamic association processes of solutes, e.g., amphiphilic molecules, and to find the inappropriate selections of representative sites on solutes in these criteria may bring about appreciable influence on the estimation of dynamic association behaviors such as unrealistic packing radii and even misleading packing structures. It would be better to select dynamically representative sites on solute molecules based on the characteristic of solute associations. Our detailed discussions give a guide on how to determine an appropriate criterion to accurately analyze the association behaviors of solute molecules in aqueous solutions.展开更多
The dependence of measured viscosity on NaCl concentration (0.1 to 3.0M), pH (range of 2—13) and cadoxen composition w_(cad) (from 2% to 100%) for the lacquer polysaccharide in NaCl/cadoxen/H_2O mixture containing HC...The dependence of measured viscosity on NaCl concentration (0.1 to 3.0M), pH (range of 2—13) and cadoxen composition w_(cad) (from 2% to 100%) for the lacquer polysaccharide in NaCl/cadoxen/H_2O mixture containing HCl or without were obtained. All the viscosity exponents γ in the Mark-Houwink equations under three different solvent condition arc close to 0.5. The w_(cad) dependence of reduced viscosity ηsp/c confirms the single strand chain of the polysaccharide. As the γ values close to 0.5 and values of unperturbed dimension <S^2>_θ/M and [η] much smaller than those for usual linear polymers, these facts suggest that the polysaccharide chains in the aqueous solutions should be dense random coil owing to the highly branched structure.展开更多
基金supported by the National Natural Science Foundation of China(22125802 and 22078010)Beijing Natural Science Foundation(2222017)Big Science Project from BUCT(XK180301)。
文摘A new type of rubidium ion-imprinted polymer has been synthesized by the surface-imprinting technique using methacrylic acid as the functional monomer,the rubidium ion as the template,methanol as the solvent,and silica as a carrier.Ethylene glycol dimethacrylate and 2,2-azobisisobutyronitrile were used as acrosslinker and an initiator,respectively.In addition,based on the macrocyclic effect of crown ethers,the 18-crown-6 ligand was introduced as a ligand to fix the template ions better.Scanning electron microscopy,zeta-potential analysis,Fourier transform infrared spectroscopy,thermogravimetric analysis,and X-ray photoelectron spectroscopy were performed to characterize the ion-imprinted polymer.The effects of the preparation and adsorption conditions on the adsorption performance of the rubidium ion-imprinted polymer were investigated.The results indicated that the rubidium ion-imprinted polymer has high selectivity and faster kinetics than other adsorbents,with an equilibrium adsorption capacity of 200.19 mg·g^(-1)at 298 K within 25 min.The sorption isotherm was well described by the Freundlich isotherm model,while the adsorption kinetics fitted the pseudo-second-order kinetic model.Consecutive adsorption-desorption experiments showed that the ion-imprinted polymer had good chemical stability and reusability.
基金supported by the Key Area Research&Development Program of Guangdong Province(2020B0101070001)the National Natural Science Foundation of China(21978053,51508547)。
文摘Levulinic acid(LA)is one of the top-12 most promising biomass-based platform chemicals,which has a wide range of applications in a variety of fields.However,separation and purification of LA from aqueous solution or actual hydrolysate continues to be a challenge.Among various downstream separation technologies,liquid-liquid extraction is a low-cost,effective,and simple process to separate LA.The key breakthrough lies in the development of extractants with high extraction efficiency,good hydrophobicity,and low cost.In this work,three hydrophobic deep eutectic solvents(DESs)based on tri-n-octylamine(TOA)as hydrogen bond acceptor(HBA)and alcohols(butanol,2-octanol,and menthol)as hydrogen bond donors(HBDs)were developed to extract LA from aqueous solution.The molar ratios of HBD and HBA,extraction temperature,contact time,solution pH,and initial LA concentration,DES/water volume ratios were systematically investigated.Compared with 2-octanol-TOA and menthol-TOA DES,the butanol-TOA DES exhibited the superior extraction performance for LA,with a maximum extraction efficiency of 95.79±1.4%.Moreover,the solution pH had a great impact on the LA extraction efficiency of butanol-TOA(molar ratio=3:1).It is worth noting that the extraction equilibrium time was less than 0.5 h.More importantly,the butanol-TOA(3:1)DES possesses good extraction abilities for low,medium,and high concentrations of LA.
基金supported by National Natural Science Foundation of China (Nos. 12075037 and 22206013)the Natural Science Foundation of Jiangsu Province (No. BK20210857)the Leading Innovative Talents Cultivation Project of Changzhou City (No. CQ20210083)。
文摘Ozone(O_(3)) generated by a dielectric barrier discharge(DBD) is widely used in various industrial processes. In this study, NaCl aqueous solution was used as a novel electric power transmission electrode in a DBD reactor(instead of a traditional metal electrode) for highly efficient ozone generation. The results demonstrated that a high O_(3) yield of 242 g k Wh^(-1) with a concentration of 14.6 g m^(-3)O_(3) was achieved. The power transmission mechanism works because NaCl aqueous solution behaves as a capacitor when an alternating pulse voltage below 8 k Hz is used.Compared with the resistance of the discharge barrier and discharge space, the resistance of NaCl aqueous solution can be ignored, which ensures that O_(3) is generated efficiently. It is expected that O_(3) generation using NaCl aqueous solution as a novel electrode in a DBD reactor could be an alternative technology with good application prospects.
基金supported by the National Natural Science Foundation of China(No.21776264).
文摘Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is proposed by using molecular dynamics simulation,and the relationship between ion-to-ion interaction and salt solubility in a simulated seawater water-salt system is investigated.By analyzing the variation of distance and contact time between ions in an electrolyte solution,from both spatial and temporal perspectives,new parameters were proposed to describe the interaction between ions:interaction distance(ID),and interaction time ratio(ITR).The best correlation between characteristic time ratio and solubility was found for a molar ratio of salt-to-water of 10:100 with a correlation coefficient of 0.96.For the same salt,a positive correlation was found between CTR and the molar ratio of salt and water.For type 1-1,type 2-1,type 1-2,and type 2-2 salts,the correlation coefficients between CTR and solubility were 0.93,0.96,0.92,and 0.98 for a salt-to-water molar ratio of 10:100,respectively.The solubility of multiple salts was predicted by simulations and compared with experimental values,yielding an average relative deviation of 12.4%.The new ion-interaction parameters offer significant advantages in describing strongly correlated and strongly hydrated electrolyte solutions.
基金The financial support from National Natural Science Foundation of China(21978096,21861132019,and 21776074)Natural Science Foundation of Shanghai(19ZR1412600)is greatly acknowledged
文摘1,5-Pentanediamine(PDA)produced by biological fermentation becomes popular,but the separation of PDA from the broth is a typical difficult problem.In this work,the performance of 200 ionic liquids(ILs),formed by combining 25 cations and 8 anions,in the extraction of PDA from aqueous solution were evaluated using COSMO-RS model.The extraction mechanism was investigated with the help ofσ-profile and interaction energy analyses.Both the cation and anion have impacts on the extraction efficiency,where cation mainly influences the interaction of IL with PDA and anion affects the hydrophobicity of IL.The IL composed of long alkyl-chain in cation and the anion of[PF6]-or[TF2 N]-,which has theσ-profile more likely distributed in the nonpolar region but less distributed in the polar region,is favorable for extraction.The experimental liquid-liquid equilibrium demonstrated the effects of cation and anion on extraction performance,which validated the reliability of COSMO-RS model in IL screening for PDA extraction.The IL[IM-1,8][PF6]could serve as a promising extractant for the downstream separation process of the biological production of PDA.
基金supported by the National Natural Science Foundation of China (40673043 and 20576073)the Program for New Century Excellent Talents in University of Ministry of Education of China (NCET-06-0088)
文摘Ionic liquids (ILs) have been regarded as the potential novel solvents for improved analytical- and process-scale separation methods.The development of methods for the recovery of ILs from aqueous solutions to escape contamination and recycle samples will ultimately govern the viability of ILs in the future industrial applications. Therefore, in this paper a new method for separation of ILs from their dilute aqueous solutions and simultaneously purification of water was proposed on the basis of the CO2 hydrate formation. For illustration, the dilute aqueous solutions with concentrations of ILs ranging from 2× 10^-3 mol% to 2×10^-1 mol% were concentrated. The results show that the separation efficiency is very impressive and that the new method is applicable to aqueous solutions of both hydrophobic and hydrophilic ILs. Compared to the literature separation method based on the supercritical CO2, the new method is applicable to lower concentrations, and more importantly, its operation condition is mild.
基金Deanship of Scientific Research(DSR)at King Saud University(KSU),Saudi Arabia for financially supporting this research project(No.RG-1435-078)。
文摘Coal fly ash(CFA)is composed of minerals containing some oxides in crystalline phase(i.e.,quartz and mullite),as well as unburned carbon as mesoporous material,thus enabling CFA to act as a dual-sites adsorbent with unique properties.This work focused on the adsorption of Pb(Ⅱ)and Zn(Ⅱ)from binary system,a mixture containing two metal ion solutions present simultaneously,onto NaOH-modified CFA(MCFA).Several adsorption tests were conducted to evaluate the effect of several parameters,including pH and contact times.The experiment results indicated that chemical treatment of CFA with NaOH increased pore volume from 0.021 to 0.223 cm^3·g^(-1).In addition,it could also enhance the availability of functional groups on both minerals and unburned carbon,resulting in almost 100%Pb(Ⅱ)and 97%Zn(Ⅱ)adsorbed.The optimum pH for adsorption system was pH=3 and quasi-equilibrium occurred in 240 minutes.Equilibrium data from the experimental results were analyzed using Modified Extended Langmuir(MEL)and Competitive Adsorption Langmuir-Langmuir(CALL)isotherm models.The analysis results showed that the CALL isotherm model could better describe the Pb(Ⅱ)and Zn(Ⅱ)adsorption process onto MCFA in binary system compared with MEL isotherm model.
基金This work was financially supported by the National Natural Science Foundation of China (Nos. 50301009 and 50171039)the Education Development Foundation of Shanghai (No. 03AK24)
文摘To investigate the degradation of corrosion resistance of Zircaloy-4 in LiOHaqueous solution, SIMS (secondary ion mass spectrometry) analysis was performed to examine theprofiles of Li^+, K^+, and OH^- in oxide layers formed in the same concentration (0.1 mol/L) LiOHand KOH solutions. Even though the oxide layers have an equal thickness, the pene-tration depth ofK^+ is shallower than that of Li^+, and the penetration depth of OH^- corroded in KOH solution isalso shal-ower than that corroded in LiOH solution. It shows that the diffusion of OH^- into oxidelayer is accompanied by the corresponding cation. The difference of degradation effect of LiOH andKOH solutions on the corrosion resistance of Zircaloy-4 was discussed.
文摘Chemical effects in different aqueous solutions induced by plasma with glow discharge electrolysis (GDE) and contact glow discharge electrolysis (CGDE) are described in this paper. The experimental and discharge characteristics are also reviewed. These are followed by a discussion of their mechanisms of both anodic and cathodic CGDE..
基金a grant from the Science and Technology Key Project of Education Ministry, China and KJCX-01 of Northwest Normal University, Chi
文摘Degradation of α-naphthol induced by plasma in aqueous solution was investigated in different initial concentration with contact glow discharge electrolysis(CGDE). The results showed that the degradation of α-naphthol obeyed the first-rate law. Some of predominant products were analyzed by a high performance liquid chromatography (HPLC). A path of α-naphthol disappearance caused by plasma was proposed according to the detected intermediate products.
基金the DREAM project of MOST,China(Grant No.2016YFC0600408)the Strategic Priority Research Program(B)of Chinese Academy of Sciences(Grant No.XDB18000000)the Program of the National Mineral Rock and Fossil Specimens Resource Center from MOST,China.
文摘Carbonate-bearing fluids widely exist in different geological settings,and play important roles in transporting some elements such as the rare earth elements.They may be trapped as large or small fluid inclusions(with the size down to<1μm sometimes),and record critical physical-chemical signals for the formations of their host minerals.Spectroscopic methods like Raman spectroscopy and infrared spectroscopy have been proposed as effective methods to quantify the carbonate concentrations of these fluid inclusions.Although they have some great technical advantages over the conventional microthermometry method,there are still some technical difficulties to overcome before they can be routinely used to solve relevant geological problems.The typical limitations include their interlaboratory difference and poor performance on micro fluid inclusions.This study prepared standard ion-distilled water and K_(2)CO_(3)aqueous solutions at different molarities(from 0.5 to 5.5 mol/L),measured densities,collected Raman and infrared spectra,and explored correlations between the K_(2)CO_(3)molarity and the spectroscopic features at ambient P-T conditions.The result confirms that the Raman O-H stretching mode can be used as an internal standard to determine the carbonate concentrations despite some significant differences among the correlations,established in different laboratories,between the relative Raman intensity of the C-O symmetric stretching mode and that of the O-H stretching mode.It further reveals that the interlaboratory difference can be readily removed by performing one high-quality calibration experiment,provided that later quantifying analyses are conducted using the same Raman spectrometer with the same analytical conditions.Our infrared absorption data were collected from thin fluid films(thickness less than~2μm)formed by pressing the prepared solutions in a Microcompression Cell with two diamond-II plates.The data show that both the O-H stretching mode and the O-H bending mode can be used as internal standards to determine the carbonate concentrations.Since the IR signals of the C-O antisymmetric stretching vibration of the CO32ion,and the O-H stretching and bending vibrations from our thin films are very strong,their relative IR absorbance intensity,if well calibrated,can be used to investigate the micron-sized carbonate-bearing aqueous fluid inclusions.This study establishes the first calibration of this kind,which may have some applications.Additionally,our spectroscopic data suggest that as the K_(2)CO_(3)concentration increases the aqueous solution forms more large water molecule clusters via more intense hydrogen-bonding.This process may significantly alter the physical and chemical behavior of the fluids.
基金Supported by the National Natural Science Foundation of China(Nos.20577014 and 41073063)
文摘We compared the photochemical reaction of m-cresol containing ·OH precursors such as H2O2, NO2 and NO3 in aqueous solution with those in ice. The results show that the conversion rate of m-cresol in aqueous solution was higher than that in ice. H2O2, NO2 and NO3 all accelerated the photoconversion of m-cresol in both aqueous solution and ice. The photochemical reactions of m-cresol obeys the first order kinetics equation. According to the photoproducts identified by GC-MS, we proposed that hydroxylation and nitration reactions occurred in both aqueous solution and ice. Coupling reaction was common in ice, however, in aqueous solution it was found only in UV system. Our results suggest that the photochemical reactions of m-cresol were different in aqueous solution and in ice.
基金supported by the Fundamental Research Funds of Shandong University(2018TB037)。
文摘The objective of this work is to contribute an understanding of the effects of electrons in the plasmas on the mass transfer of plasma species in aqueous solution by means of the numerical simulation based on a one-dimensional diffusion-reaction model.The plasma species are divided into two groups,i.e.electrons and the other species,and the mass transfer in the three scenarios has been simulated,including the systematic calculations of the depth distributions of five major reactive species,OH,O3,HO2,O2^-,and H2O2.In the three scenarios,the particles considered to enter into aqueous solution are all the plasma species(the scenario Ⅰ,where the mass transfer of plasma species is a result due to the synergy of the electrons and the other plasma species),the other species(the scenario Ⅱ),and only electrons in plasma species(the scenario Ⅲ),respectively.The detailed analyses on the difference between the depth distributions of each reactive species in these three scenarios show the following conclusions.The electrons play an important role in the mass transfer of plasma species in aqueous solution and the synergy of the electrons and the other plasma species(the electron-species synergy)presents its different effects on the mass transfer.The vast majority of H2O2 are generated from a series of the electronrelated reactions in aqueous solution,which is hardly affected by the electron-species synergy.Compared to the results when only the electrons enter into the liquid region,the electron-species synergy evidently weakens the generation of O2^-,O3,and OH,but promotes to produce HO2.
基金Project supported by the National Natural Science Foundation of China (20101006)Nano Technology Special Foundationof Shanghai Science and Technology Committee (0452nm073) and Shanghai Education Committee
文摘Agglomeration-free nanosized ZrO2-HfO2-Y2O3-Sc2O3 composite powders were successfully synthesized by Sol-Gel technique in heated aqueous solution of alcohol, using analytically pure ZrOCl2 · 8H2O, HfOCl2·8H2O, Y(NO3)3·6H2O, and Sc2O3 as raw materials. The effect of synthesis condition on the size and dispersity of the composite powders was investigated by means of XRD, TEM, and TG-DSC techniques. The results showed that well-dispersed predecessor of ZrO2-HfO2-Y2O3-Sc2O3 composite nanopowders could be obtained. The optional condition : PEG6000 as dispersant was 1%, alcohol/H2O ratio was 5/1, metallic ion concentration in whole solution was 0.5 mol·L^-1 and the pH value of the solution was 12. After calcined at 620 ℃, the powder obtained was in uniform cubic structure, and its average particle size was about 13 nm, which was good for producing nanocrystalline solid electrolyte.
基金Supported by the National Natural Science Foundation of China(21729601,21776123)the Doctoral Program of Higher Education(20133221110001)+1 种基金the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the Kempe Foundations,and Swedish Energy Agency(P40548-1).
文摘In this work,an air-blast atomizing column was used to study the CO2 capture performance with aqueous MEA(mono-ethanol-amine)and Na OH solutions.The effects of gas flow rate,the liquid to gas ratio(L/G),the CO2 concentration on the CO2 removal efficiency(η)and the volumetric overall mass transfer coefficient(KGav)were investigated.The air-blast atomizing column was also compared with the pressure spray tower on the studies of the CO2 capture performance.For the aqueous MEA and Na OH solutions,the experimental results show that theηdecreases with increasing gas flow rate and CO2 concentration while it increases with increasing L/G.The effects on KGavare more complicated than those forη.When the CO2 concentration is low(3 vol%),KGavincreases with increasing gas flow rate while decreases with increasing L/G.However,when the CO2 concentration is high(9.5 vol%),as the gas flow rate and L/G increases,KGavincreases first and then decreases.The aqueous MEA solution achieves higherηand KGavthan the aqueous Na OH solution.The air-blast atomizing column shows a good performance on CO2 capture.
文摘The reverse osmosis (RO) separation of aqueous organic solutions, such as alcohols, amines, aldehydes, acids, ketones, and esters etc., by PAA (polyacrylic acid)/PSF (polysulfone) composite membrane has been studied. It was found that the separation results for aliphatic alcohols, amines and aldehydes are satisfactory, the solute rejection (R-a) and the volume fluxes of solutions (J(V)) for 1000 ppm ethanol, ethylamine and ethyl aldehyde are 66.2%, 61.0%, 84.0% and 0.90 x 10(-6), 0.35 x 10(-6), 0.40 X 10(-6) m(3)/m(2) . s, respectively, at 5.0 MPa and 30 degrees C. R-a increased with increasing molecular weights of alcohols, amines and aldehydes, and the R-a for n-amyl alcohol, n-butylamine and n-butyl aldehyde reached 94.3%, 88.6% and 96.0%, respectively. Satisfactory separation results (R-a > 70%) for ketones, esters, phenols and polyols have been obtained with the PAA/PSF composite membrane. The effect of operating pressure on the properties of reverse osmosis has also been investigated. Analysis of experimental data with Spiegler-Kedem's transport model has been carried out and the membrane constants such as reflection coefficient sigma, solute and hydraulic permeabilities omega and L-p for several organic solutes have been obtained.
基金financially supported by grants from the National Natural Science Foundation of China(No.31500493)the Liaoning Educational Common Scientific Research Project(No.L2015044)+1 种基金the Liaoning Natural Science Foundation(No.2015020576)the Open Foundation of the Key Lab of Pulp and Paper Science & Technology,and Ministry of Education(Shandong Province),Qilu University of Technology(No.08031338)
文摘Quaternized cellulose( QC) derivatives were synthesized by reacting cellulose with 3-chloro-2-hydroxypropyl trimethyl ammonium chloride( CHPTAC) in an aqueous solution of Na OH-urea. The chemical structures and physical properties of the obtained QC derivatives were characterized using nitrogen content analysis,Fourier transform infrared spectroscopy( FT-IR),~1H-nuclear magnetic resonance(1H-NMR),X-ray diffraction( XRD),and thermal gravity analysis( TGA). The FT-IR and ~1H-NMR results confirmed the successful introduction of cationic quaternary ammonium groups into the main chain of cellulose. A series of QC derivatives with the degree of substitution( DS) values ranging from 0. 33 to 0. 80 were derived by adjusting the molar ratio of CHPTAC to anhydroglucose unit( AGU) of cellulose,concentration of cellulose in the Na OH-urea solution,as well as reaction temperature and time. According to the DS values of the QC derivatives,the optimized synthetic conditions were as follows: 25℃ reaction temperature,3% cellulose in Na OH-urea solution,the molar ratio of etherification agent to glycosidic cellulose of 15∶ 1,and 12 h reaction time. The TGA and XRD results revealed that the crystalline structure was destroyed during etherification,and the thermal stability of the QC derivatives was lower than that of cellulose.
基金financially supported by the National Key Research and Development Program of China (2017YFA0208200)the National Natural Science Foundation of China (52102100,22022505 and 21872069)+4 种基金the Natural Science Foundation of Jiangsu Province (BK20181469)Guangdong Basic and Applied Basic Research Foundation (2020A1515110035)the Fundamental Research Funds for the Central Universities (0205-14380266,0205-14380272)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province (BK20220008)the 2021 Suzhou Gusu Leading Talents of Science and Technology Innovation and Entrepreneurship in Wujiang District。
文摘To solve the environmental pollution and low yield during the sythesis of zeolitic imidazolate frameworks(ZIFs)and their derived materials,a KOH-assisted aqueous strategy is proposed to synthesize cobalt zeolitic imidazolate framework(ZIF-67)polyhedrons,which are used as precursors to prepare cobalt selenide/carbon composites with different crystal phases(Co_(0.85)Se,CoSe_2).When evaluated as anode material for lithium ion batteries,Co_(0.85)Se/C composites deliver a reversible capacity of 758.7 m A·h·g^(-1)with a capacity retention rate of 90.5%at 1.0 A·g^(-1)after 500 cycles,and the superior rate capability is 620 m A·h·g^(-1)at 2.0 A·g^(-1).The addition of KOH accelerates the production of ZIF-67 crystals by boosting deprotonation of dimethylimidazole,resulting in rapid growth and structures transition from two-dimensional to three-dimensional of ZIF-67 in aqueous solution,which greatly promotes the application of MOFs in the field of energy storage and conversion.
基金Supported by the National Science Fund for Outstanding Young Scholars under Grant No 11422542the Key Research Program of Chinese Academy of Sciences under Grant No KJZD-EW-M03,KIPCAS+1 种基金the Shanghai Supercomputer Center of Chinathe High Performance Computing Center of Shanghai University
文摘How to determine accurately the association states of solutes in aqueous systems is of fundamental importance in a variety of chemical, physical, and biological processes, We apply four widely used criteria to analyze the dynamic association processes of solutes, e.g., amphiphilic molecules, and to find the inappropriate selections of representative sites on solutes in these criteria may bring about appreciable influence on the estimation of dynamic association behaviors such as unrealistic packing radii and even misleading packing structures. It would be better to select dynamically representative sites on solute molecules based on the characteristic of solute associations. Our detailed discussions give a guide on how to determine an appropriate criterion to accurately analyze the association behaviors of solute molecules in aqueous solutions.
文摘The dependence of measured viscosity on NaCl concentration (0.1 to 3.0M), pH (range of 2—13) and cadoxen composition w_(cad) (from 2% to 100%) for the lacquer polysaccharide in NaCl/cadoxen/H_2O mixture containing HCl or without were obtained. All the viscosity exponents γ in the Mark-Houwink equations under three different solvent condition arc close to 0.5. The w_(cad) dependence of reduced viscosity ηsp/c confirms the single strand chain of the polysaccharide. As the γ values close to 0.5 and values of unperturbed dimension <S^2>_θ/M and [η] much smaller than those for usual linear polymers, these facts suggest that the polysaccharide chains in the aqueous solutions should be dense random coil owing to the highly branched structure.