Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(...Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(KOH:anthracite= 1:1), modified by melamine or urea and then treated at 1173 K to obtain the modified carbons.The porous structure, the chemical composition and the electrochemical characteristics of the carbons were investigated by nitrogen sorption, XPS and electrochemical methods respectively.Electrochemical experiments were performed in an organic electrolytic solution of 1 M(C2H5)4NBF4/PC.The samples modified by the different methods showed differences in chemical composition that introduced varying degrees of electrochemical performance enhancement.The presence of nitrogen enhanced the electron donor properties and the surface wettability of the activated carbons:this ensured a sufficient utilization of the exposed surface for charge storage.展开更多
Interaction of anionic polyelectrolyte with cationic gemini surfactant has been investigated by coarse-grained molecular dynamics simulation.Polyelectrolyte facilitates the oppositely charged ionic surfactants to aggr...Interaction of anionic polyelectrolyte with cationic gemini surfactant has been investigated by coarse-grained molecular dynamics simulation.Polyelectrolyte facilitates the oppositely charged ionic surfactants to aggregate by suppressing the electrostatic repulsion between ionic head groups leading to the formation of micellar complex.With addition of surfactant,the conformation of polyion chain changes from stretched to random coiled to spherical,and at the same time more free micelles are formed by surfactants in mixtures.Increasing the length of spacer or tail chain in gemini surfactant will weaken its interaction with polyelectrolyte and simultaneously strengthen its tendency to self-assemble.The simulation results are consistent with experimental observations and reveal that the electrostatic interaction plays an important role in the interaction of polyelectrolyte with gemini sur- factant.展开更多
As the structure of electrical double layer(EDL)is crucial for the transport properties of ions in micro/nanochannels,to demonstrate the effects of the ion-ion correlations on EDL structures in mixture electrolyte sol...As the structure of electrical double layer(EDL)is crucial for the transport properties of ions in micro/nanochannels,to demonstrate the effects of the ion-ion correlations on EDL structures in mixture electrolyte solutions,the interaction forces between two mica surfaces immersed in different volume fractions of LaCl3/KCl and LaCl3/MgCl2 mixture solutions with a total ionic strength of 10^-4 mol/L were measured using a surface forces apparatus(SFA).The results reveal that the surface charge of mica surfaces can be inversed at a critical concentration of La^3+ions in electrolyte solutions,due to the correlations between La^3+ions.The addition of monovalent has negligible effects on ion-ion correlations,while the charge inversion was slightly suppressed by introducing the divalent ions.The mechanism of charge inversion in mixture electrolyte solutions was analyzed based on the strongly correlated liquid(SCL)theory.These findings provide implications for understanding the effects of ion-ion correlations on EDL structures,surface charge properties,and ion transportation.展开更多
Electrostatic separation is one of the mineral processing methods based on mineral conductivity.This method has some significant problems such as being sensitive to humidity,high middling product,and impurity of non-c...Electrostatic separation is one of the mineral processing methods based on mineral conductivity.This method has some significant problems such as being sensitive to humidity,high middling product,and impurity of non-conductive minerals.In this study,a new pretreatment method was proposed for the separation of zircon from quartz before electrostatic separation to solve these disadvantages.In this regard,two stages of pretreatment were applied which involved using collector of sodium dodecyl sulfate(SDS)for adjusting wettability of the zircon surface and spraying electrolyte aqueous solution to increase conductivity of the quartz surface.The effects of important parameters including pH,collector concentration,conditioning time,and concentration and type of electrolyte on the process efficiency were evaluated.The results showed that the optimal conditions of high-tension electrical separation were pH of 4,SDS concentration of 1×10-4 mol/L,conditioning time of 4 min and NaCl as an electrolyte with concentration of 4.27 mol/L.Separation efficiency of 95.12% was achieved in optimum conditions.This pretreatment method can be successfully used before high-tension electrical separation to separate the conductive or non-conductive minerals with various compositions.展开更多
Polyelectrolyte becomes more and more popular in electrocatalysis.The understanding of electrode/polyelectrolyte interfaces at the molecular level is important for guiding further the polyelectrolyte-based electrocata...Polyelectrolyte becomes more and more popular in electrocatalysis.The understanding of electrode/polyelectrolyte interfaces at the molecular level is important for guiding further the polyelectrolyte-based electrocatalysis.Herein,we demonstrate an in-situ surface-enhanced Raman spectroscopic method by using a three-electrode spectroelectrochemical cell towards characterizing the electrode/polyelectrolyte interfaces.The Ag/AgCl and Ag/Ag_(2)O electrodes are used as the reference electrode in the acidic and the alkaline systems,respectively.The working electrode is made of a transparent carbon thin film which loads the electrocatalysts.The applications of this method are demonstrated through the in-situ characterizations of the p-methylthiophenol adsorbed on the Au and Pt and the electrochemical oxidation of Au on polyelectrolyte membranes.The potential-dependent spectral features of these two systems show that this method is a powerful tool for investigating the electrode/polyelectrolyte interfaces in electrocatalysis.展开更多
This study is to understand the impact of operating condition, especially initial operation temperature （Tini） which is set in high temperature range, on the temperature profile of the interface between PEM （polyme...This study is to understand the impact of operating condition, especially initial operation temperature （Tini） which is set in high temperature range, on the temperature profile of the interface between PEM （polymer electrolyte membrane） and catalyst layer at the cathode （i.e., the reaction surface） in a single PEFC （polymer electrolyte fuel cell）. A 1D multi-plate heat transfer model based on the temperature data of separator measured using thermograph in a power generation experiment was developed to evaluate the reaction surface temperature （Treact）. This study investigated the effects of flow rate, relative humidity and type of supply gas as well as Tini on the temperature distribution on reaction surface. The results obtained in 02 supply case show that, the temperature rise at the segments near the outlet of cell decreases with increasing Tini irrespective of relative humidity of supply gas （RH）, while it is not seen in air supply case. Regarding the segments except near the outlet in 02 supply case, Treact - Tini increases with increasing Tini for 40% RH. The temperature distribution on reaction surface in 02 supply case is wider with increasing Tini as well as decreasing RH, though that in air supply case is relatively even.展开更多
Interaction between beta-lactum antibiotic drug ciprofloxacin hydrochloride(CFH)and cationic surfactant cetyltrimethylammonium bromide(CTAB)was performed conductometrically in aqueous as well as in the occurrence of d...Interaction between beta-lactum antibiotic drug ciprofloxacin hydrochloride(CFH)and cationic surfactant cetyltrimethylammonium bromide(CTAB)was performed conductometrically in aqueous as well as in the occurrence of different salts(NaCl,KCl as well as NH_4Cl)over the temperature range of 298.15–323.15 K at the regular interval of 5 K.CFH drug has been suggested for the treatment of bacterial infections such as urinary tract infections and acute sinusitis.A clear critical micelle concentration(CMC)was obtained for pure CTAB as well as(CFH+CTAB)mixed systems.The decrease in CMC values of CTAB caused by the addition of CFH reveals the existence of the interaction between the components and therefore it is the indication of micelle formation at lower concentration of CTAB and their CMC values further decrease in attendance of salts.A nonlinear behavior in the CMC versus T plot was observed in all the cases.The ΔG_m^0 values are found to be negative in present study systems demonstrated the stability of the solution.The values of ΔH_m^0 and ΔS_m^0 reveal the existence of hydrophobic and electrostatic interactions between CFH and CTAB.The thermodynamic properties of transfer for the micellization were also evaluated and discussed in detail.Molecular dynamic simulation disclosed that environment of water and salts have impact on the hydrophobic interaction between CFH and CTAB.In water and salts,CTAB adopts spherical micelle in which charged hydrophilic groups are interacted with waters whereas hydrophobic tails form the core of the micelle.This hydrophobic core region is highly conserved and protected.In addition,micelle formation is more favorable in aqueous Na Cl solution than other solutions.展开更多
Experiments on proton dissociation from the surfaces of goethite, amorphous Al oxide, kaolinite and latosolwere carried out, showing amphoteric behavior with reactions of proton dissociation-association on the surface...Experiments on proton dissociation from the surfaces of goethite, amorphous Al oxide, kaolinite and latosolwere carried out, showing amphoteric behavior with reactions of proton dissociation-association on the surfaces andbuffering capacity in such a sequence as amorphous Al oxide > latosol > kaolinite > goethite. Dissociation con-stants of surface proton, pK_(sa) are significantly correlated with surface charge density, which has been proved with anelectrochemical model. Tbe intrinsic constants of proton dissociation, K_(sa)(int), gained by extrapolation to zero charconditions of plots of pK_(sa) against σ_o, could be used to estimate the acidity strength of variable charge surfaces. Thevalue of pK_(sa)(int) is 8.08 for goethite, 1 .2 for amorphous Al oxide, 6.62 for kaolinite and 5 .32 for latosol.展开更多
The streaming potential of poly（vinyl butyral） （PVB） hollow fiber membrane was studied in different electrolyte solutions （including NaCl, KCl, CaCl2 and MgCl2）, the effects of ionic strength, ion valence and pH...The streaming potential of poly（vinyl butyral） （PVB） hollow fiber membrane was studied in different electrolyte solutions （including NaCl, KCl, CaCl2 and MgCl2）, the effects of ionic strength, ion valence and pH value on the streaming potential （SP） of the membrane were investigated. The zeta potentials and surface charge densities of the membrane were estimated on the basis of Helmholtz-Smoluchowski equation and Gouy-Chapmann theory. The results show that the PVB membrane has a weak negative charge due to the specific adsorption of ions. Moreover, the streaming potential, the zeta potential and the surface charge density of the membrane depend strongly on the salt concentration and the type and valence of ions. The iso-electric point （IEP） of the PVB membrane is arotmd 3.0 in the monovalent media （NaC1 and KC1） and 3.5 in divalent electrolytes （CaCl2 and MgCl2）. A few retentions were obtained for PVB membrane in low concentration solutions. This result verifies that the negative charged membrane surface can reject inorganic solutes by means of electrostatic repulsion effect even though the size of membrane pores is much larger than the size of salts.展开更多
The purpose of this study is to verify an 1D multi-plate heat-transfer model estimating the temperature distribution on the interface between polymer electrolyte membrane and catalyst layer at cathode in single cell o...The purpose of this study is to verify an 1D multi-plate heat-transfer model estimating the temperature distribution on the interface between polymer electrolyte membrane and catalyst layer at cathode in single cell of polymer electrolyte fuel cell, which is named as reaction surface in this study, with a 3D numerical simulation model solving many governing equations on the coupling phenomena in the cell. The results from both models/simulations agreed well. The effects of initial operation temperature, flow rate, and relative humidity of supply gas on temperature distribution on the reaction surface were also investigated. It was found in both 1D and 3D simulations that, the temperature rise （i.e., Treact-Tini） of the reaction surface from initial operation temperature at 70℃ was higher than that at 80℃ irrespective of flow rate of supply gas. The effect of relative humidity of supply gas on Treact- Tini near the inlet of the cell was small. Compared to the previous studies conducted under the similar operation conditions, the Treact - Tini calculated by 1D multi-plate heat-transfer model in this study as well as numerical simulation using 3D model was reasonable.展开更多
A series of porous carbon materials with wide range of specific surface areas and different heteroatom contents had been prepared using polyaniline as carbon precursor and KOH as an activating agent. Effect of surface...A series of porous carbon materials with wide range of specific surface areas and different heteroatom contents had been prepared using polyaniline as carbon precursor and KOH as an activating agent. Effect of surface area and heteroatom of porous carbon materials on specific capacitance was investigated thoroughly in two typical aqueous KOH and organic 1-butyl-3- methylimidazolium tetrafluoroborate/acetonitirle electrolytes. The different trends of capacitance performance were observed in these two electrolytes. Electrochemical analyses suggested that the presence of faradaic interactions on heteroatom-enriched carbon materials in organic environment is less significant than that observed in aqueous electrolytes. Thus, in aqueous electrolyte, a balance between surface area and heteroatom content of activated porous carbon would be found to develop a supercapacitor with high energy density. In organic electrolyte, the capacitance performance of porous carbon is strongly dependent on the surface area. The results may be useful for the design of porous carbon-based supercapacitor with the desired capacitive performance in aqueous and organic electrolytes.展开更多
基金Projects 50672025 and 50730003 supported by the National Natural Science Foundation of China
文摘Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(KOH:anthracite= 1:1), modified by melamine or urea and then treated at 1173 K to obtain the modified carbons.The porous structure, the chemical composition and the electrochemical characteristics of the carbons were investigated by nitrogen sorption, XPS and electrochemical methods respectively.Electrochemical experiments were performed in an organic electrolytic solution of 1 M(C2H5)4NBF4/PC.The samples modified by the different methods showed differences in chemical composition that introduced varying degrees of electrochemical performance enhancement.The presence of nitrogen enhanced the electron donor properties and the surface wettability of the activated carbons:this ensured a sufficient utilization of the exposed surface for charge storage.
基金Supported by the National Natural Science Foundation of China （No.20476025）, the Doctoral Research Foundation of the Ministry of Education of China （No.20050251004）, E-institute of Shanghai High Institution Grid （No.200303） and Shanghai Municipal Science and Technology Commission of China （No.05DJ14002）.
文摘Interaction of anionic polyelectrolyte with cationic gemini surfactant has been investigated by coarse-grained molecular dynamics simulation.Polyelectrolyte facilitates the oppositely charged ionic surfactants to aggregate by suppressing the electrostatic repulsion between ionic head groups leading to the formation of micellar complex.With addition of surfactant,the conformation of polyion chain changes from stretched to random coiled to spherical,and at the same time more free micelles are formed by surfactants in mixtures.Increasing the length of spacer or tail chain in gemini surfactant will weaken its interaction with polyelectrolyte and simultaneously strengthen its tendency to self-assemble.The simulation results are consistent with experimental observations and reveal that the electrostatic interaction plays an important role in the interaction of polyelectrolyte with gemini sur- factant.
基金The National Natural Science Foundation of China(No.51605090)the Natural Science Foundation of Jiangsu Province(No.BK20160776,BK20160670)Research Foundation of Nanjing Institute of Technology(No.YKJ201502)。
文摘As the structure of electrical double layer(EDL)is crucial for the transport properties of ions in micro/nanochannels,to demonstrate the effects of the ion-ion correlations on EDL structures in mixture electrolyte solutions,the interaction forces between two mica surfaces immersed in different volume fractions of LaCl3/KCl and LaCl3/MgCl2 mixture solutions with a total ionic strength of 10^-4 mol/L were measured using a surface forces apparatus(SFA).The results reveal that the surface charge of mica surfaces can be inversed at a critical concentration of La^3+ions in electrolyte solutions,due to the correlations between La^3+ions.The addition of monovalent has negligible effects on ion-ion correlations,while the charge inversion was slightly suppressed by introducing the divalent ions.The mechanism of charge inversion in mixture electrolyte solutions was analyzed based on the strongly correlated liquid(SCL)theory.These findings provide implications for understanding the effects of ion-ion correlations on EDL structures,surface charge properties,and ion transportation.
文摘Electrostatic separation is one of the mineral processing methods based on mineral conductivity.This method has some significant problems such as being sensitive to humidity,high middling product,and impurity of non-conductive minerals.In this study,a new pretreatment method was proposed for the separation of zircon from quartz before electrostatic separation to solve these disadvantages.In this regard,two stages of pretreatment were applied which involved using collector of sodium dodecyl sulfate(SDS)for adjusting wettability of the zircon surface and spraying electrolyte aqueous solution to increase conductivity of the quartz surface.The effects of important parameters including pH,collector concentration,conditioning time,and concentration and type of electrolyte on the process efficiency were evaluated.The results showed that the optimal conditions of high-tension electrical separation were pH of 4,SDS concentration of 1×10-4 mol/L,conditioning time of 4 min and NaCl as an electrolyte with concentration of 4.27 mol/L.Separation efficiency of 95.12% was achieved in optimum conditions.This pretreatment method can be successfully used before high-tension electrical separation to separate the conductive or non-conductive minerals with various compositions.
文摘Polyelectrolyte becomes more and more popular in electrocatalysis.The understanding of electrode/polyelectrolyte interfaces at the molecular level is important for guiding further the polyelectrolyte-based electrocatalysis.Herein,we demonstrate an in-situ surface-enhanced Raman spectroscopic method by using a three-electrode spectroelectrochemical cell towards characterizing the electrode/polyelectrolyte interfaces.The Ag/AgCl and Ag/Ag_(2)O electrodes are used as the reference electrode in the acidic and the alkaline systems,respectively.The working electrode is made of a transparent carbon thin film which loads the electrocatalysts.The applications of this method are demonstrated through the in-situ characterizations of the p-methylthiophenol adsorbed on the Au and Pt and the electrochemical oxidation of Au on polyelectrolyte membranes.The potential-dependent spectral features of these two systems show that this method is a powerful tool for investigating the electrode/polyelectrolyte interfaces in electrocatalysis.
文摘This study is to understand the impact of operating condition, especially initial operation temperature （Tini） which is set in high temperature range, on the temperature profile of the interface between PEM （polymer electrolyte membrane） and catalyst layer at the cathode （i.e., the reaction surface） in a single PEFC （polymer electrolyte fuel cell）. A 1D multi-plate heat transfer model based on the temperature data of separator measured using thermograph in a power generation experiment was developed to evaluate the reaction surface temperature （Treact）. This study investigated the effects of flow rate, relative humidity and type of supply gas as well as Tini on the temperature distribution on reaction surface. The results obtained in 02 supply case show that, the temperature rise at the segments near the outlet of cell decreases with increasing Tini irrespective of relative humidity of supply gas （RH）, while it is not seen in air supply case. Regarding the segments except near the outlet in 02 supply case, Treact - Tini increases with increasing Tini for 40% RH. The temperature distribution on reaction surface in 02 supply case is wider with increasing Tini as well as decreasing RH, though that in air supply case is relatively even.
文摘Interaction between beta-lactum antibiotic drug ciprofloxacin hydrochloride(CFH)and cationic surfactant cetyltrimethylammonium bromide(CTAB)was performed conductometrically in aqueous as well as in the occurrence of different salts(NaCl,KCl as well as NH_4Cl)over the temperature range of 298.15–323.15 K at the regular interval of 5 K.CFH drug has been suggested for the treatment of bacterial infections such as urinary tract infections and acute sinusitis.A clear critical micelle concentration(CMC)was obtained for pure CTAB as well as(CFH+CTAB)mixed systems.The decrease in CMC values of CTAB caused by the addition of CFH reveals the existence of the interaction between the components and therefore it is the indication of micelle formation at lower concentration of CTAB and their CMC values further decrease in attendance of salts.A nonlinear behavior in the CMC versus T plot was observed in all the cases.The ΔG_m^0 values are found to be negative in present study systems demonstrated the stability of the solution.The values of ΔH_m^0 and ΔS_m^0 reveal the existence of hydrophobic and electrostatic interactions between CFH and CTAB.The thermodynamic properties of transfer for the micellization were also evaluated and discussed in detail.Molecular dynamic simulation disclosed that environment of water and salts have impact on the hydrophobic interaction between CFH and CTAB.In water and salts,CTAB adopts spherical micelle in which charged hydrophilic groups are interacted with waters whereas hydrophobic tails form the core of the micelle.This hydrophobic core region is highly conserved and protected.In addition,micelle formation is more favorable in aqueous Na Cl solution than other solutions.
文摘Experiments on proton dissociation from the surfaces of goethite, amorphous Al oxide, kaolinite and latosolwere carried out, showing amphoteric behavior with reactions of proton dissociation-association on the surfaces andbuffering capacity in such a sequence as amorphous Al oxide > latosol > kaolinite > goethite. Dissociation con-stants of surface proton, pK_(sa) are significantly correlated with surface charge density, which has been proved with anelectrochemical model. Tbe intrinsic constants of proton dissociation, K_(sa)(int), gained by extrapolation to zero charconditions of plots of pK_(sa) against σ_o, could be used to estimate the acidity strength of variable charge surfaces. Thevalue of pK_(sa)(int) is 8.08 for goethite, 1 .2 for amorphous Al oxide, 6.62 for kaolinite and 5 .32 for latosol.
基金Project(21176264)supported by the National Natural Science Foundation of ChinaProject(11JJ2010)supported by the Hunan Provincial Natural Science Foundation of China+1 种基金Project(CL11096)supported by the Undergraduate Innovation Training Foundation of Central South University,ChinaProject(BL12053)supported by the Undergraduate Innovation Training Foundation of Hunan Province,China
文摘The streaming potential of poly（vinyl butyral） （PVB） hollow fiber membrane was studied in different electrolyte solutions （including NaCl, KCl, CaCl2 and MgCl2）, the effects of ionic strength, ion valence and pH value on the streaming potential （SP） of the membrane were investigated. The zeta potentials and surface charge densities of the membrane were estimated on the basis of Helmholtz-Smoluchowski equation and Gouy-Chapmann theory. The results show that the PVB membrane has a weak negative charge due to the specific adsorption of ions. Moreover, the streaming potential, the zeta potential and the surface charge density of the membrane depend strongly on the salt concentration and the type and valence of ions. The iso-electric point （IEP） of the PVB membrane is arotmd 3.0 in the monovalent media （NaC1 and KC1） and 3.5 in divalent electrolytes （CaCl2 and MgCl2）. A few retentions were obtained for PVB membrane in low concentration solutions. This result verifies that the negative charged membrane surface can reject inorganic solutes by means of electrostatic repulsion effect even though the size of membrane pores is much larger than the size of salts.
文摘The purpose of this study is to verify an 1D multi-plate heat-transfer model estimating the temperature distribution on the interface between polymer electrolyte membrane and catalyst layer at cathode in single cell of polymer electrolyte fuel cell, which is named as reaction surface in this study, with a 3D numerical simulation model solving many governing equations on the coupling phenomena in the cell. The results from both models/simulations agreed well. The effects of initial operation temperature, flow rate, and relative humidity of supply gas on temperature distribution on the reaction surface were also investigated. It was found in both 1D and 3D simulations that, the temperature rise （i.e., Treact-Tini） of the reaction surface from initial operation temperature at 70℃ was higher than that at 80℃ irrespective of flow rate of supply gas. The effect of relative humidity of supply gas on Treact- Tini near the inlet of the cell was small. Compared to the previous studies conducted under the similar operation conditions, the Treact - Tini calculated by 1D multi-plate heat-transfer model in this study as well as numerical simulation using 3D model was reasonable.
基金supported by the Top Hundred Talents Program of Chinese Academy of Sciencesthe National Natural Science Foundation of China(21203223)the Youth Science Foundation of Gansu Province(1107RJYA274)
文摘A series of porous carbon materials with wide range of specific surface areas and different heteroatom contents had been prepared using polyaniline as carbon precursor and KOH as an activating agent. Effect of surface area and heteroatom of porous carbon materials on specific capacitance was investigated thoroughly in two typical aqueous KOH and organic 1-butyl-3- methylimidazolium tetrafluoroborate/acetonitirle electrolytes. The different trends of capacitance performance were observed in these two electrolytes. Electrochemical analyses suggested that the presence of faradaic interactions on heteroatom-enriched carbon materials in organic environment is less significant than that observed in aqueous electrolytes. Thus, in aqueous electrolyte, a balance between surface area and heteroatom content of activated porous carbon would be found to develop a supercapacitor with high energy density. In organic electrolyte, the capacitance performance of porous carbon is strongly dependent on the surface area. The results may be useful for the design of porous carbon-based supercapacitor with the desired capacitive performance in aqueous and organic electrolytes.
