Human life quality requires both industrial/agricultural fast development and high environmental quality.However,the two aspects are conflicted as some contaminants are accidentally released into the environment,poten...Human life quality requires both industrial/agricultural fast development and high environmental quality.However,the two aspects are conflicted as some contaminants are accidentally released into the environment,potentially harmful to human health even at extra-low concentrations.展开更多
Aqueous zinc(Zn)-ion batteries(AZIBs)have gained significant interest in energy storage due to several unique advantages.Utilizing waterbased electrolytes enhances environmental sustainability,while the abundance and ...Aqueous zinc(Zn)-ion batteries(AZIBs)have gained significant interest in energy storage due to several unique advantages.Utilizing waterbased electrolytes enhances environmental sustainability,while the abundance and affordability of Zn offer economic benefits.Manganese(Mn)-based materials,commonly used as cathodes in these batteries,provide high theoretical capacity,high electrical conductivity,and good structural stability.However,these materials suffer from capacity degradation over repeated cycles due to structural collapse and limited conductivity.To address this problem,we synthesized a magnesium(Mg)-and Mn-based composite,Mg^(2+)-Mn_(3)O_(4),using the hydrothermal method with an optimized amount of ammonium hydroxide(NH_(4)OH)solution.This approach effectively stabilizes the structure during cycling,enhancing both capacity retention and conductivity.The Zn^(2+)/H+intercalation/deintercalation process was confirmed by experimental results and ex-situ X-ray diffraction analysis,which demonstrates that Mg^(2+),along with optimized NH_(4)OH amount,prevents structural collapse and improves conductivity.Under optimal process conditions,the composite electrode(Mg^(2+)-Mn_(3)O_(4)–8 ml)achieved a capacity of 173.58 mA h g^(-1) at 0.5 A g^(-1),with excellent rate performance of 71.39 mA h g^(-1) at 10 A g^(-1).Remarkably,even at 5 A g^(-1),the electrode maintained a capacity of 86.87 mA h g^(-1) over 2100 cycles,underscoring the role of Mg^(2+)and NH_(4)OH in enhancing the reversible insertion/extraction stability of Zn^(2+)in Mn-based layered materials.This study presents a novel strategy for metal-ion incorporation in Mn-based AZIBs,offering insights into the optimization of cathode materials and advancing research on associated storage mechanisms.展开更多
In recent years,with the rapid developme nt of the econo my and society,pollution of valuable metal ions in wastewater has become a major challenge to environmental sustainability.In order to solve the pollution cause...In recent years,with the rapid developme nt of the econo my and society,pollution of valuable metal ions in wastewater has become a major challenge to environmental sustainability.In order to solve the pollution caused by metal ions,researchers have conducted continuous re searches and explored various re mediation methods.Crown ether has attracted great attention because of its ionic radius and cavity size matching well with metal ions,which makes it have the ability to selectively complex metal ions.This unique property enables the directed removal and recovery of metal ions and makes crown ethers increasingly popular in extraction and separation processes.In this paper,the research progress of crown ethers in the extraction and separation of valuable metal ions was reviewed,with emphasis on the principles,extraction systems and the key factors affecting the extraction process.This study can provide some technical support for the application of separation and extraction of valuable metal ions by crown ether.展开更多
A novel adsorbent was prepared from granular red mud mixed with cement and its potential to be a suitable adsorbent for the removal of cadmium ions from aqueous solutions was evaluated. The wet red mud was directly mi...A novel adsorbent was prepared from granular red mud mixed with cement and its potential to be a suitable adsorbent for the removal of cadmium ions from aqueous solutions was evaluated. The wet red mud was directly mixed up with cement at different mass fractions of 2%-8% and their properties were investigated. Based on the textural characteristics and strength, the granular red mud with 2% addition of cement maintaining for 6 d is identified to have better properties. The batch adsorption experiments for adsorption of Cd2+ ions from solution were performed at 30, 40 and 50 °C at different initial concentrations under the condition of constant pH of 6.5. The equilibrium adsorption was found to increase with the increase of temperature during the adsorption process. Langmuir adsorption isotherm model was found to match the experimental adsorption isotherm better. The kinetics of adsorption was modeled using a pseudo second order kinetic model and the model parameters were estimated.展开更多
A solution cooling absorption（SCA）approach is proposed to modify the aqueous ammonia absorption refrigerat-ion cycle using the strong solution from the absorber to cool the forepart of the absorption in the cycle fo...A solution cooling absorption（SCA）approach is proposed to modify the aqueous ammonia absorption refrigerat-ion cycle using the strong solution from the absorber to cool the forepart of the absorption in the cycle for reclaiming some portion of absorption heat.As a consequence of raised temperature at the inlet,the strong solution partially boils at the outlet of the solution heat exchanger,and diminishes the thermal heat consumption of the heat source.The calculation results show that the coefficient of performance（COP）of this modified cycle is about 28.3% higher than that of the traditional cycle under typical conditions;while the required heat transfer area of the total heat exchangers of the cycle is somewhat less than that of the traditional one.The capacity of refrigeration with the new absorption cycle is more than doubled in contrast to the adsorption scheme with an identical configuration.It is sufficient to supply a fishing boat the chilling capacity for preservation of fishing products with the modified cycle chiller driven by its diesel engine exhaust.展开更多
A universal thermodynamic model of calculating mass action concentrations for structural units or ion couples in ternary and binary strong electrolyte aqueous solution was developed based on the ion and molecule coexi...A universal thermodynamic model of calculating mass action concentrations for structural units or ion couples in ternary and binary strong electrolyte aqueous solution was developed based on the ion and molecule coexistence theory and verified in four kinds of binary aqueous solutions and two kinds of ternary aqueous solutions. The calculated mass action concentrations of structural units or ion couples in four binary aqueous solutions and two ternary solutions at 298.15 K have good agreement with the reported activity data from literatures after shifting the standard state and concentration unit. Therefore, the calculated mass action concentrations of structural units or ion couples from the developed universal thermodynamic model for ternary and binary aqueous solutions can be applied to predict reaction ability of components in ternary and binary strong electrolyte aqueous solutions. It is also proved that the assumptions applied in the developed thermodynamic model are correct and reasonable, i.e., strong electrolyte aqueous solution is composed of cations and anions as simple ions, H2O as simple molecule and other hydrous salt compounds as complex molecules. The calculated mass action concentrations of structural units or ion couples in ternary and binary strong electrolyte aqueous solutions strictly follow the mass action law.展开更多
Cu nanoparticles were prepared by reducing Cu2＋ ions with ascorbic acid through aqueous solution reduction method. The effects of solution pH and average size of Cu2O particles on the preparation of Cu nanoparticles ...Cu nanoparticles were prepared by reducing Cu2＋ ions with ascorbic acid through aqueous solution reduction method. The effects of solution pH and average size of Cu2O particles on the preparation of Cu nanoparticles were investigated. Cu particles were prepared at pH 3, 5 or 7, with the smallest Cu particles obtained at pH 7. However, Cu particles could not be prepared at pH 9 or 11. The average size of Cu2O particles can affect that of Cu particles. Larger Cu2O particles result in larger Cu particles. In addition, experiments were conducted to explore the reaction process by measuring the X-ray diffraction （XRD） patterns of specimens collected at different time points during the reaction. It was found that Cu（OH）2 was initially formed as a precursor, followed by the formation of Cu2O, which was finally reduced to Cu particles.展开更多
The preparation of Cu nanoparticles by the aqueous solution reduction method was investigated. The effects of different reaction parameters on the preparation of Cu nanoparticles were studied. The optimum conditions f...The preparation of Cu nanoparticles by the aqueous solution reduction method was investigated. The effects of different reaction parameters on the preparation of Cu nanoparticles were studied. The optimum conditions for preparing well-dispersed nanoparticles were found as follows: 0.4 mol/L NaBH4 was added into solution containing 0.2 mol/L Cu2+, 1.0% gelatin dispersant in mass fraction, and 1.2 mol/L NH3?H2O at pH 12 and 313 K. In addition, a series of experiments were performed to discover the reaction process. NH3?H2O was found to be able to modulate the reaction process. At pH=10, Cu2+ was transformed to Cu(NH3)42+ as precursor after the addition of NH3?H2O, and then Cu(NH3)42+ was reduced by NaBH4 solution. At pH=12, Cu2+ was transformed to Cu(OH)2 as precursor after the addition of NH3?H2O, and Cu(OH)2 was then reduced by NaBH4 solution.展开更多
All-atom molecular dynamics （MD） simulation and the NMR spectra are used to investigate the interactions in N-glycylglycine aqueous solution. Different types of atoms exhibit different capability in forming hydrogen...All-atom molecular dynamics （MD） simulation and the NMR spectra are used to investigate the interactions in N-glycylglycine aqueous solution. Different types of atoms exhibit different capability in forming hydrogen bonds by the radial distribution function analysis. Some typical dominant aggregates are found in different types of hydrogen bonds by the statistical hydrogen-bonding network. Moreover, temperature-dependent NMR are used to compare with the results of the MD simulations. The chemical shifts of the three hydrogen atoms all decrease with the temperature increasing which reveals that the hydrogen bonds are dominant in the glycylglycine aqueous solution. And the NMR results show agreement with the MD simulations. All-atom MD simulations and NMR spectra are successful in revealing the structures and interactions in the N-glycylglycine-water mixtures.展开更多
All-atom molecular simulations and two-dimensional nuclear overhauser effect spectrum have been used to study the conformations of carnosine in aqueous solution. Intramolecular distances, root-mean-square deviation, r...All-atom molecular simulations and two-dimensional nuclear overhauser effect spectrum have been used to study the conformations of carnosine in aqueous solution. Intramolecular distances, root-mean-square deviation, radius of gyration, and solvent-accessible surface are used to characterize the properties of the carnosine. Carnosine can shift between extended and folded states, but exists mostly in extended state in water. Its preference for extension in pure water has been proven by the 2D nuclear magnetic resonance （NMR） experiment. The NMR experimental results are consistent with the molecular dynamics simulations.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
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
Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate i...Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate ion concentration is studied.A novel kinetic model for the α-radiolysis of nitric acid aqueous solution is established,by considering the direct and indirect effects.The simulation results agree well with the experimental data,indicating the validity of our model to treat the reaction paths for generation and consumption of nitrous acid.It is shown that the redox reactions involving Pu cannot be neglected in theα-radiolysis of the solution.The results provide a better understanding of the α-ray radiolysis of aqueous nitric acid.展开更多
As the abundant biopolymer, cellulose can be used as a feedstock for chemicals and materials. Effective conversion of cellulose by simple processes is a key point. Degradation of cellulose in its homogeneous solution ...As the abundant biopolymer, cellulose can be used as a feedstock for chemicals and materials. Effective conversion of cellulose by simple processes is a key point. Degradation of cellulose in its homogeneous solution is attractive for the molecular chains are free and spread. Here,microcrystalline cellulose was first dissolved in aqueous solution of Na OH and urea, and then hydrothermal reaction was carried out at various temperature and time. Fluorescence carbon dots(CDs) were generated accompanied with six organic acids: oxalic acid, formic acid, malonic acid, lactic acid, acetic acid, and fumaric acid. The yields of all organic acids and CDs, and the fluorescence quantum yield(QY) of CDs were studied at different reaction conditions. It was found that the maximum yield of organic acids and CDs are 80.1% and 6.03%, respectively, and the highest QY of the CDs is 10.9%. Fluorescence studies reveal that the as-prepared CDs has efficient selectivity and sensitivity toward iron ions in acidic condition, indicating it is a potential fluorescent sensor to the detection of Fe3+. Importantly, it provides a panorama to summary the degradation routes of cellulose in its homogeneous aqueous solution with both organic molecules and CDs as products.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
A novel Ni（Ⅱ） ion-imprinted silica gel polymer was prepared via the surface imprinting technique combined with aqueous solution polymerization by using 2-acrylamido-2-methyl-1-propanesulfonic acid（AMPS） as a func...A novel Ni（Ⅱ） ion-imprinted silica gel polymer was prepared via the surface imprinting technique combined with aqueous solution polymerization by using 2-acrylamido-2-methyl-1-propanesulfonic acid（AMPS） as a functional monomer for the selective separation of Ni（Ⅱ） from aqueous solution. The sorbent showed good chemical and thermal stability. Kinetics studies indicated that the equilibrium adsorption was achieved within 10 min and the adsorption kinetics fitted well with the pseudo-second-order kinetic model. The maximum adsorption capacity of the ion-imprinted polymer towards Ni（Ⅱ） at the optimal p H of 7.0 was 66.22 mg·g^（-1）. The relative selectivity coefficients of the sorbent were 9.23, 15.71, 14.72 and 20.15 for Ni（Ⅱ）/Co（Ⅱ）, Ni（Ⅱ）/Cu（Ⅱ）, Ni（Ⅱ）/Zn（Ⅱ） and Ni（Ⅱ）/Pb（Ⅱ）, respectively. The adsorption isotherm fitted well with Langmuir isotherm model. The thermodynamic results indicated that the adsorption of Ni（Ⅱ） was a spontaneous and endothermic process. The sorbent showed good reusability evidenced by six cycles of adsorption/desorption experiments. The precision of this method is satisfactory. Thus, the prepared sorbent can be considered as a promising sorbent for selective separation of Ni（Ⅱ） in real water samples.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
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
Density, pH, viscosity, conductivity and the Raman spectra of aqueous NaB（OH）4 solutions precisely measured as functions of concentration at different temperatures （293.15, 298.15, 303.15, 313.15 and 323.15 K） are...Density, pH, viscosity, conductivity and the Raman spectra of aqueous NaB（OH）4 solutions precisely measured as functions of concentration at different temperatures （293.15, 298.15, 303.15, 313.15 and 323.15 K） are presented. Polyborate distributions in aqueous NaB（OH）4 solution were calculated, covering all the concentration range, B（OH）4 is the most dominant species, other polyborate anions are less than 5.0%. The volumetric and the transport properties were discussed in detail, both of these properties indicate that B（OH）4 behaves as a struc- ture-disordered anion.展开更多
1H NMR chemical shifts of binary aqueous mixtures of acylamide, alcohol, dimethyl sulphoxide (DMSO), and acetone are correlated by statistical associating fluid theory (SAFT) association model. The comparison between ...1H NMR chemical shifts of binary aqueous mixtures of acylamide, alcohol, dimethyl sulphoxide (DMSO), and acetone are correlated by statistical associating fluid theory (SAFT) association model. The comparison between SAPT association model and Wilson equation shows that the former is better for dealing with aqueous solutions. Finally, the specialties of both models are discussed.展开更多
基金supported by National Natural Science Foundation of China(No.U21A20290)。
文摘Human life quality requires both industrial/agricultural fast development and high environmental quality.However,the two aspects are conflicted as some contaminants are accidentally released into the environment,potentially harmful to human health even at extra-low concentrations.
基金supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2018R1A6A1A03025708).
文摘Aqueous zinc(Zn)-ion batteries(AZIBs)have gained significant interest in energy storage due to several unique advantages.Utilizing waterbased electrolytes enhances environmental sustainability,while the abundance and affordability of Zn offer economic benefits.Manganese(Mn)-based materials,commonly used as cathodes in these batteries,provide high theoretical capacity,high electrical conductivity,and good structural stability.However,these materials suffer from capacity degradation over repeated cycles due to structural collapse and limited conductivity.To address this problem,we synthesized a magnesium(Mg)-and Mn-based composite,Mg^(2+)-Mn_(3)O_(4),using the hydrothermal method with an optimized amount of ammonium hydroxide(NH_(4)OH)solution.This approach effectively stabilizes the structure during cycling,enhancing both capacity retention and conductivity.The Zn^(2+)/H+intercalation/deintercalation process was confirmed by experimental results and ex-situ X-ray diffraction analysis,which demonstrates that Mg^(2+),along with optimized NH_(4)OH amount,prevents structural collapse and improves conductivity.Under optimal process conditions,the composite electrode(Mg^(2+)-Mn_(3)O_(4)–8 ml)achieved a capacity of 173.58 mA h g^(-1) at 0.5 A g^(-1),with excellent rate performance of 71.39 mA h g^(-1) at 10 A g^(-1).Remarkably,even at 5 A g^(-1),the electrode maintained a capacity of 86.87 mA h g^(-1) over 2100 cycles,underscoring the role of Mg^(2+)and NH_(4)OH in enhancing the reversible insertion/extraction stability of Zn^(2+)in Mn-based layered materials.This study presents a novel strategy for metal-ion incorporation in Mn-based AZIBs,offering insights into the optimization of cathode materials and advancing research on associated storage mechanisms.
基金financially supported by the National Natural Science Foundation of China (52174336)the Natural Science Foundation of Shandong Province (ZR2021MB051)。
文摘In recent years,with the rapid developme nt of the econo my and society,pollution of valuable metal ions in wastewater has become a major challenge to environmental sustainability.In order to solve the pollution caused by metal ions,researchers have conducted continuous re searches and explored various re mediation methods.Crown ether has attracted great attention because of its ionic radius and cavity size matching well with metal ions,which makes it have the ability to selectively complex metal ions.This unique property enables the directed removal and recovery of metal ions and makes crown ethers increasingly popular in extraction and separation processes.In this paper,the research progress of crown ethers in the extraction and separation of valuable metal ions was reviewed,with emphasis on the principles,extraction systems and the key factors affecting the extraction process.This study can provide some technical support for the application of separation and extraction of valuable metal ions by crown ether.
基金Project (51264022) supported by the National Natural Science Foundation of China
文摘A novel adsorbent was prepared from granular red mud mixed with cement and its potential to be a suitable adsorbent for the removal of cadmium ions from aqueous solutions was evaluated. The wet red mud was directly mixed up with cement at different mass fractions of 2%-8% and their properties were investigated. Based on the textural characteristics and strength, the granular red mud with 2% addition of cement maintaining for 6 d is identified to have better properties. The batch adsorption experiments for adsorption of Cd2+ ions from solution were performed at 30, 40 and 50 °C at different initial concentrations under the condition of constant pH of 6.5. The equilibrium adsorption was found to increase with the increase of temperature during the adsorption process. Langmuir adsorption isotherm model was found to match the experimental adsorption isotherm better. The kinetics of adsorption was modeled using a pseudo second order kinetic model and the model parameters were estimated.
基金The National Natural Science Foundation of China(No.50776016)the National Key Technology R&D Program of China during the 11th Five-Year Plan Period(No.2008BAJ12B02)
文摘A solution cooling absorption（SCA）approach is proposed to modify the aqueous ammonia absorption refrigerat-ion cycle using the strong solution from the absorber to cool the forepart of the absorption in the cycle for reclaiming some portion of absorption heat.As a consequence of raised temperature at the inlet,the strong solution partially boils at the outlet of the solution heat exchanger,and diminishes the thermal heat consumption of the heat source.The calculation results show that the coefficient of performance（COP）of this modified cycle is about 28.3% higher than that of the traditional cycle under typical conditions;while the required heat transfer area of the total heat exchangers of the cycle is somewhat less than that of the traditional one.The capacity of refrigeration with the new absorption cycle is more than doubled in contrast to the adsorption scheme with an identical configuration.It is sufficient to supply a fishing boat the chilling capacity for preservation of fishing products with the modified cycle chiller driven by its diesel engine exhaust.
基金Project supported by Publication Foundation of National Science and Technology Academic Books of China
文摘A universal thermodynamic model of calculating mass action concentrations for structural units or ion couples in ternary and binary strong electrolyte aqueous solution was developed based on the ion and molecule coexistence theory and verified in four kinds of binary aqueous solutions and two kinds of ternary aqueous solutions. The calculated mass action concentrations of structural units or ion couples in four binary aqueous solutions and two ternary solutions at 298.15 K have good agreement with the reported activity data from literatures after shifting the standard state and concentration unit. Therefore, the calculated mass action concentrations of structural units or ion couples from the developed universal thermodynamic model for ternary and binary aqueous solutions can be applied to predict reaction ability of components in ternary and binary strong electrolyte aqueous solutions. It is also proved that the assumptions applied in the developed thermodynamic model are correct and reasonable, i.e., strong electrolyte aqueous solution is composed of cations and anions as simple ions, H2O as simple molecule and other hydrous salt compounds as complex molecules. The calculated mass action concentrations of structural units or ion couples in ternary and binary strong electrolyte aqueous solutions strictly follow the mass action law.
文摘Cu nanoparticles were prepared by reducing Cu2＋ ions with ascorbic acid through aqueous solution reduction method. The effects of solution pH and average size of Cu2O particles on the preparation of Cu nanoparticles were investigated. Cu particles were prepared at pH 3, 5 or 7, with the smallest Cu particles obtained at pH 7. However, Cu particles could not be prepared at pH 9 or 11. The average size of Cu2O particles can affect that of Cu particles. Larger Cu2O particles result in larger Cu particles. In addition, experiments were conducted to explore the reaction process by measuring the X-ray diffraction （XRD） patterns of specimens collected at different time points during the reaction. It was found that Cu（OH）2 was initially formed as a precursor, followed by the formation of Cu2O, which was finally reduced to Cu particles.
文摘The preparation of Cu nanoparticles by the aqueous solution reduction method was investigated. The effects of different reaction parameters on the preparation of Cu nanoparticles were studied. The optimum conditions for preparing well-dispersed nanoparticles were found as follows: 0.4 mol/L NaBH4 was added into solution containing 0.2 mol/L Cu2+, 1.0% gelatin dispersant in mass fraction, and 1.2 mol/L NH3?H2O at pH 12 and 313 K. In addition, a series of experiments were performed to discover the reaction process. NH3?H2O was found to be able to modulate the reaction process. At pH=10, Cu2+ was transformed to Cu(NH3)42+ as precursor after the addition of NH3?H2O, and then Cu(NH3)42+ was reduced by NaBH4 solution. At pH=12, Cu2+ was transformed to Cu(OH)2 as precursor after the addition of NH3?H2O, and Cu(OH)2 was then reduced by NaBH4 solution.
文摘All-atom molecular dynamics （MD） simulation and the NMR spectra are used to investigate the interactions in N-glycylglycine aqueous solution. Different types of atoms exhibit different capability in forming hydrogen bonds by the radial distribution function analysis. Some typical dominant aggregates are found in different types of hydrogen bonds by the statistical hydrogen-bonding network. Moreover, temperature-dependent NMR are used to compare with the results of the MD simulations. The chemical shifts of the three hydrogen atoms all decrease with the temperature increasing which reveals that the hydrogen bonds are dominant in the glycylglycine aqueous solution. And the NMR results show agreement with the MD simulations. All-atom MD simulations and NMR spectra are successful in revealing the structures and interactions in the N-glycylglycine-water mixtures.
文摘All-atom molecular simulations and two-dimensional nuclear overhauser effect spectrum have been used to study the conformations of carnosine in aqueous solution. Intramolecular distances, root-mean-square deviation, radius of gyration, and solvent-accessible surface are used to characterize the properties of the carnosine. Carnosine can shift between extended and folded states, but exists mostly in extended state in water. Its preference for extension in pure water has been proven by the 2D nuclear magnetic resonance （NMR） experiment. The NMR experimental results are consistent with the molecular dynamics simulations.
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(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partly supported by the National Natural Science Foundation of China(No.21377122)
文摘Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate ion concentration is studied.A novel kinetic model for the α-radiolysis of nitric acid aqueous solution is established,by considering the direct and indirect effects.The simulation results agree well with the experimental data,indicating the validity of our model to treat the reaction paths for generation and consumption of nitrous acid.It is shown that the redox reactions involving Pu cannot be neglected in theα-radiolysis of the solution.The results provide a better understanding of the α-ray radiolysis of aqueous nitric acid.
基金supported by the National Natural Science Foundation of China (No. 51373162 and 51673180)
文摘As the abundant biopolymer, cellulose can be used as a feedstock for chemicals and materials. Effective conversion of cellulose by simple processes is a key point. Degradation of cellulose in its homogeneous solution is attractive for the molecular chains are free and spread. Here,microcrystalline cellulose was first dissolved in aqueous solution of Na OH and urea, and then hydrothermal reaction was carried out at various temperature and time. Fluorescence carbon dots(CDs) were generated accompanied with six organic acids: oxalic acid, formic acid, malonic acid, lactic acid, acetic acid, and fumaric acid. The yields of all organic acids and CDs, and the fluorescence quantum yield(QY) of CDs were studied at different reaction conditions. It was found that the maximum yield of organic acids and CDs are 80.1% and 6.03%, respectively, and the highest QY of the CDs is 10.9%. Fluorescence studies reveal that the as-prepared CDs has efficient selectivity and sensitivity toward iron ions in acidic condition, indicating it is a potential fluorescent sensor to the detection of Fe3+. Importantly, it provides a panorama to summary the degradation routes of cellulose in its homogeneous aqueous solution with both organic molecules and CDs as products.
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.
文摘A novel Ni（Ⅱ） ion-imprinted silica gel polymer was prepared via the surface imprinting technique combined with aqueous solution polymerization by using 2-acrylamido-2-methyl-1-propanesulfonic acid（AMPS） as a functional monomer for the selective separation of Ni（Ⅱ） from aqueous solution. The sorbent showed good chemical and thermal stability. Kinetics studies indicated that the equilibrium adsorption was achieved within 10 min and the adsorption kinetics fitted well with the pseudo-second-order kinetic model. The maximum adsorption capacity of the ion-imprinted polymer towards Ni（Ⅱ） at the optimal p H of 7.0 was 66.22 mg·g^（-1）. The relative selectivity coefficients of the sorbent were 9.23, 15.71, 14.72 and 20.15 for Ni（Ⅱ）/Co（Ⅱ）, Ni（Ⅱ）/Cu（Ⅱ）, Ni（Ⅱ）/Zn（Ⅱ） and Ni（Ⅱ）/Pb（Ⅱ）, respectively. The adsorption isotherm fitted well with Langmuir isotherm model. The thermodynamic results indicated that the adsorption of Ni（Ⅱ） was a spontaneous and endothermic process. The sorbent showed good reusability evidenced by six cycles of adsorption/desorption experiments. The precision of this method is satisfactory. Thus, the prepared sorbent can be considered as a promising sorbent for selective separation of Ni（Ⅱ） in real water samples.
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.
基金Supported by the National Natural Science Foundation of China （20873172） and Main Direction Program of Knowledge In- novation of Chinese Academy of Sciences （KZCX2-EW-307）.
文摘Density, pH, viscosity, conductivity and the Raman spectra of aqueous NaB（OH）4 solutions precisely measured as functions of concentration at different temperatures （293.15, 298.15, 303.15, 313.15 and 323.15 K） are presented. Polyborate distributions in aqueous NaB（OH）4 solution were calculated, covering all the concentration range, B（OH）4 is the most dominant species, other polyborate anions are less than 5.0%. The volumetric and the transport properties were discussed in detail, both of these properties indicate that B（OH）4 behaves as a struc- ture-disordered anion.
基金Supported by the National Natural Science Foundation of China (No. 29976035)the Natural Science Foundation of Zhejiang Provincial (No. RC01051).
文摘1H NMR chemical shifts of binary aqueous mixtures of acylamide, alcohol, dimethyl sulphoxide (DMSO), and acetone are correlated by statistical associating fluid theory (SAFT) association model. The comparison between SAPT association model and Wilson equation shows that the former is better for dealing with aqueous solutions. Finally, the specialties of both models are discussed.
