This paper describes a novel method for the degradation of eosin by using glow discharge electrolysis (GDE). The effects of various parameters on the removal efficiency were studied. It was found that the eosin degr...This paper describes a novel method for the degradation of eosin by using glow discharge electrolysis (GDE). The effects of various parameters on the removal efficiency were studied. It was found that the eosin degradation could be raised considerably by increasing the applied voltage and the initial concentration, or by decreasing pH of the aqueous solution. Fe^2+ ion had an evident accelerating effect on the eosin degradation. The degradation process of eosin obeyed a pseudo-first-order reaction. The relationship between the degradation rate constant k and the reaction temperature T could be expressed by Arrhenius equation with which the apparent activation energy Ea of 14.110 kJ· mol^-1 and the pre-exponential factor k0 of 2.065× 10^-1 min^-1 were obtained, too. The determination of hydroxyl radical was carried out by using N, N-dimethyl -p-nitrosoaniline (RNO) as a scavenger. The results showed that the hydroxyl radical plays an important role in the degradation process.展开更多
Contact glow discharge electrolysis is a non-Faradaic electrochemical process with an abnormal relationship between the current and voltage. Hydroxyl radicals, hydrogen radicals and hydrogen peroxide can be produced u...Contact glow discharge electrolysis is a non-Faradaic electrochemical process with an abnormal relationship between the current and voltage. Hydroxyl radicals, hydrogen radicals and hydrogen peroxide can be produced under the glow discharge, which are often used to degrade organic contaminants in aqueous solution. In this study, with 4-nitrophenol taken as an example of contaminants and tert-butanol as a scavenger of hydroxyl radicals, the role of energetic species in degrading organic compounds was examined in detail. Moreover, the effects of the applied voltage, solution conductivity and pH on the formation of three energetic species were also observed. The formation rate constants of the three energetic species were calculated based on the experimental data.展开更多
A highly absorptive resin poly (butyl methacrylate (BMA)-co-butyl acrylate (BA)) was prepared by emulsion polymerization, which was initiated by glow discharge electrolysis plasma (GDEP). The effects of discha...A highly absorptive resin poly (butyl methacrylate (BMA)-co-butyl acrylate (BA)) was prepared by emulsion polymerization, which was initiated by glow discharge electrolysis plasma (GDEP). The effects of discharge voltage, discharge time, monomer ratio and the amounts of cross- linking agent were examined and discussed in detaiI. The chemical structure of the obtained resin was characterized by means of attenuated total reflectance Fourier transform infrared spectroscopy, thermogravimetric analysis, and scanning electron microscopy. The optimal conditions were ob- tained as: discharge voltage was 600 V, discharge time was 8 min, the ratios of BMA:BA being 2:1 for chloroform and 3:1 for xylene, with 2% N, N'-methylenebis. Under optimal conditions, the oil absorbency was 70 g/g for chloroform and 46 g/g for xylene. Moreover, the absorptive dynamical behavior of the resulting resin was also investigated.展开更多
Contact glow discharge electrolysis of some chloroanilines in sodium sulfate was investigated in different initial concentrations. Each of them underwent the dechlorination, deam-ination through oxidative degradation,...Contact glow discharge electrolysis of some chloroanilines in sodium sulfate was investigated in different initial concentrations. Each of them underwent the dechlorination, deam-ination through oxidative degradation, and were eventually decomposed into hydrogen carbonate and carbon dioxide. It was testified that the chlorine atom and amidogen could be transformed into chloride ion and nitrite ion, respectively. Fe2+ has a remarkable catalytic effect on the degradation of them. On the basis of the detailed analysis of the intermediate products and kinetic behaviors, the reaction pathway was proposed, in which the attack of hydroxyl radical on the benzene ring of starting material might be a key step.展开更多
In this paper, we use methyl violet as a model organic substrate in wastewater to study the effect of Fe(Ⅱ) ion on the contact glow discharge electrolysis (CGDE). The decoloration rate and the COD (Chemical Oxyg...In this paper, we use methyl violet as a model organic substrate in wastewater to study the effect of Fe(Ⅱ) ion on the contact glow discharge electrolysis (CGDE). The decoloration rate and the COD (Chemical Oxygen Demand) value have been examined. It is found that the presence of Fe(Ⅱ) ion can accelerate obviously the degradation of methyl violet, because it reacts with H2O2 in the CGDE process to yield hydroxyl radical, just acting as a Fenton-like reagent. Moreover, the optimal conditions for decoloring methyl violet were obtained, by means of an orthogonal experiment, to be [Fe^2+] =1×10^-3 mol/L, applied voltage of 700 V of and pH = 9.0.展开更多
Glow discharge electrolysis provides an alternative method for the removal of arsenite from water. Glow discharge electrolysis of aqueous solution containing arsenite is studied under altemating current altemating cur...Glow discharge electrolysis provides an alternative method for the removal of arsenite from water. Glow discharge electrolysis of aqueous solution containing arsenite is studied under altemating current altemating current (50 Hz) discharge. It is found that arsenite [As(III)] get converted to arsenate [As(V)]. The yield is studied with various parameters such as discharge current, duration of discharge and pH (2-10). The results are interpreted on the basis of interaction of the OH and eaq (produced consequent to the interaction of H2O+ and e with water at the surface of the solution) with arsenite [As(III)] through the intermediate oxidation state, namely [As(IV)].展开更多
The oxidative degradation of 4-chlorophenol (4-CP) in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined ...The oxidative degradation of 4-chlorophenol (4-CP) in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined by high performance liquid chromatography (HPLC). Various influencing factors such as the initial pH, the concentration of 4-CP and the catalytic action of Fe^2+ were examined. The results indicate that 4-CP is eventually degraded into inorganic ion, dioxide carbon and water. The attack of hydroxyl radicals on the benzene rings of 4-CP in the initial stage of oxidative reactions is presumed to be a key step. They also suggest that the reaction is of a pseudo-first order kinetic reaction and the proposed method is an efficient way for the 4-CP degradation,展开更多
Exhaustive mineralization of pentachlorophenolate ion(PCP) in phosphate buffer was carried out using anodic contact glow discharge electrolysis(CGDE),in which plasma was sustained between the electrolyte and anode...Exhaustive mineralization of pentachlorophenolate ion(PCP) in phosphate buffer was carried out using anodic contact glow discharge electrolysis(CGDE),in which plasma was sustained between the electrolyte and anode.During CGDE,PCP degraded smoothly.The amount of total organic carbon decreased significantly,indicating the eventual conversion of the carbon atoms of benzene nucleus to inorganic carbons.Furthermore,chlorine atoms in PCP were liberated as chloride ions.As a primary intermediate product,2,3,5,6tetrachloro-1,4-benzoquinone was detected,and oxalate and formate as byproducts were also found.It was revealed that disappearance of PCP obeyed first-order kinetics.The reaction rate was generally unaffected by both O2 and inert gases in the cell,although it decreased by raising initial pH of solution.In addition,a plausible reaction pathway involving hydroxyl radical was proposed.展开更多
Destruction of 4-phenolsulfonic acid (4-PSA) in water was carded out using anodic contact glow discharge electrolysis. Accompanying the decay of 4-PSA, the amount of total organic carbon (TOC) in water correspondi...Destruction of 4-phenolsulfonic acid (4-PSA) in water was carded out using anodic contact glow discharge electrolysis. Accompanying the decay of 4-PSA, the amount of total organic carbon (TOC) in water correspondingly decreased, while the sulfonate group of 4- PSA was released as sulfate ion. Oxalate and formate were obtained as minor by-products. Additionally, phenol, 1,4-hydroquinone, hydroxyquinol and 1,4-benzoquinone were detected as primary intermediates in the initial stages of decomposition of 4-PSA. A reaction pathway involving successive attacks of hydroxyl and hydrogen radicals was assumed on the basis of the observed products and kinetics. It was revealed that the decay of both 4-PSA and TOC obeyed a first-order rate law. The effects of different Fe ions and initial concentrations of 4-PSA on the degradation rate were investigated. It was found that the presence of Fe ions could increase the degradation rate of 4-PSA, while initial concentrations lower than 80 mmol/L had no significant effect on kinetic behaviour. The disappearance rate of 4-PSA was significantly affected by pH.展开更多
In an aqueous solution, normal electrolysis at high voltages switches over spontaneously to glow discharge electrolysis and gives rise to hydroxyl radical, hydrogen peroxide, and aqueous electron, as well as several o...In an aqueous solution, normal electrolysis at high voltages switches over spontaneously to glow discharge electrolysis and gives rise to hydroxyl radical, hydrogen peroxide, and aqueous electron, as well as several other active species. Hydroxyl radical directly attacks organic contaminants to make them oxidized. In the present paper, 2-naphthylamine is eventually degraded into hydrogen carbonate and carbon dioxide. The degradation process is analyzed by using an Ultraviolet (UV) absorption spectrum, high-performance liquid chromatography (HPLC) and chemical oxygen demand (COD). It is demonstrated that 2-naphthylamine (co =30 mg·1-1) is completely converted within 2h at 30℃ and 600 V by glow discharge electrolysis, and the degradation is strongly dependent upon the presence of ferrous ions. COD is ascended in the absence of ferrous ions and descended in the presence of them.展开更多
Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that...Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that the degradation followed the first order kinetic law; Fe2+ had a remarkable catalytic effect on the removal rate of o-chloropenol. In the presence of Fe2+, 2-CP underwent an exhaustive degradation, from which the major intermediates included o-dihydroxybenze, p-hydroxybenze, p-benzoquione and carboxlic acids.展开更多
The application and characteristics of relatively big volume plasma produced with cathodic glow discharges taking place across a gaseous envelope over the cathode which was dipped into electrolyte in hydrogen generati...The application and characteristics of relatively big volume plasma produced with cathodic glow discharges taking place across a gaseous envelope over the cathode which was dipped into electrolyte in hydrogen generation were studied. A critical investigation of the influence of methanol concentration and voltage across the circuit on the composition and power consumption per cubic meter of cathode liberating gas was carried out. The course of plasma under-liquid electrolysis has the typical characteristics of glow discharge electrolysis. The cathode liberating gas was in substantial excess of the Faraday law value. When the voltage across the circuit was equal to 550 V,the volume of cathodic gas with sodium carbonate solution was equal to 16.97 times the Faraday law value. The study showed that methanol molecules are more active than water molecules. The methanol molecules were decomposed at the plasma-catholyte interface by the radicals coming out the plasma mantle. Energy consumption per cubic meter of cathodic gases (WV) decreased while methanol concentration of the electrolytes increased. When methanol concentration equaled 5% (-),WV was 10.381×103 kJ/m3,less than the corresponding theoretic value of conventional water electrolysis method. The cathodic liberating gas was a mixture of hydrogen,carbon dioxide and carbon monoxide with over 95% hydrogen,if methanol concentration was more than 15% (-). The present research work revealed an innovative application of glow discharge and a new highly efficient hydrogen generation method,which depleted less resource and energy than normal electrolysis and is environmentally friendly.展开更多
基金the Key Projects of Science and Technology of Education Ministry(00250)the Natural Science Foundation of Gansu Province(3ZS041-A25-028)+1 种基金the Projects of KJCXGC-01,NWNUCansu Key Lab of Polymer Materials,China
文摘This paper describes a novel method for the degradation of eosin by using glow discharge electrolysis (GDE). The effects of various parameters on the removal efficiency were studied. It was found that the eosin degradation could be raised considerably by increasing the applied voltage and the initial concentration, or by decreasing pH of the aqueous solution. Fe^2+ ion had an evident accelerating effect on the eosin degradation. The degradation process of eosin obeyed a pseudo-first-order reaction. The relationship between the degradation rate constant k and the reaction temperature T could be expressed by Arrhenius equation with which the apparent activation energy Ea of 14.110 kJ· mol^-1 and the pre-exponential factor k0 of 2.065× 10^-1 min^-1 were obtained, too. The determination of hydroxyl radical was carried out by using N, N-dimethyl -p-nitrosoaniline (RNO) as a scavenger. The results showed that the hydroxyl radical plays an important role in the degradation process.
基金the Key Project of Science and Technology of Education Ministry(00250)the Natural Science Foundation of Gansu Province(3ZS041-A25-028)+1 种基金the Invention Project of Science & Technology of NWNU(KJCXGC-01)Gansu Key Lab of Polymer Materials,China.
文摘Contact glow discharge electrolysis is a non-Faradaic electrochemical process with an abnormal relationship between the current and voltage. Hydroxyl radicals, hydrogen radicals and hydrogen peroxide can be produced under the glow discharge, which are often used to degrade organic contaminants in aqueous solution. In this study, with 4-nitrophenol taken as an example of contaminants and tert-butanol as a scavenger of hydroxyl radicals, the role of energetic species in degrading organic compounds was examined in detail. Moreover, the effects of the applied voltage, solution conductivity and pH on the formation of three energetic species were also observed. The formation rate constants of the three energetic species were calculated based on the experimental data.
基金supported in part by the Basic Project of Science and Research of Colleges and Universities of Gansu Province,China(5001-109)the Natural Science Foundation of Gansu Province,China(Nos.1010 RJZA015,096RJZA120)
文摘A highly absorptive resin poly (butyl methacrylate (BMA)-co-butyl acrylate (BA)) was prepared by emulsion polymerization, which was initiated by glow discharge electrolysis plasma (GDEP). The effects of discharge voltage, discharge time, monomer ratio and the amounts of cross- linking agent were examined and discussed in detaiI. The chemical structure of the obtained resin was characterized by means of attenuated total reflectance Fourier transform infrared spectroscopy, thermogravimetric analysis, and scanning electron microscopy. The optimal conditions were ob- tained as: discharge voltage was 600 V, discharge time was 8 min, the ratios of BMA:BA being 2:1 for chloroform and 3:1 for xylene, with 2% N, N'-methylenebis. Under optimal conditions, the oil absorbency was 70 g/g for chloroform and 46 g/g for xylene. Moreover, the absorptive dynamical behavior of the resulting resin was also investigated.
基金The project supported by a grant from Key Project of Science and Technology of Education Ministry, China (No. 00250) the program of KJCXGC-01, NWNU, China
文摘Contact glow discharge electrolysis of some chloroanilines in sodium sulfate was investigated in different initial concentrations. Each of them underwent the dechlorination, deam-ination through oxidative degradation, and were eventually decomposed into hydrogen carbonate and carbon dioxide. It was testified that the chlorine atom and amidogen could be transformed into chloride ion and nitrite ion, respectively. Fe2+ has a remarkable catalytic effect on the degradation of them. On the basis of the detailed analysis of the intermediate products and kinetic behaviors, the reaction pathway was proposed, in which the attack of hydroxyl radical on the benzene ring of starting material might be a key step.
基金supported in part by the Project of Key Science and Technology of Education Ministry (00250)the Natural Science Foundation of Gansu Province (3ZS041-A25- 028)the Invention Project of Science &: Technology of NWNU (KJCXGC-01), and Gansu Key Lab of Polymer Materials, China
文摘In this paper, we use methyl violet as a model organic substrate in wastewater to study the effect of Fe(Ⅱ) ion on the contact glow discharge electrolysis (CGDE). The decoloration rate and the COD (Chemical Oxygen Demand) value have been examined. It is found that the presence of Fe(Ⅱ) ion can accelerate obviously the degradation of methyl violet, because it reacts with H2O2 in the CGDE process to yield hydroxyl radical, just acting as a Fenton-like reagent. Moreover, the optimal conditions for decoloring methyl violet were obtained, by means of an orthogonal experiment, to be [Fe^2+] =1×10^-3 mol/L, applied voltage of 700 V of and pH = 9.0.
文摘Glow discharge electrolysis provides an alternative method for the removal of arsenite from water. Glow discharge electrolysis of aqueous solution containing arsenite is studied under altemating current altemating current (50 Hz) discharge. It is found that arsenite [As(III)] get converted to arsenate [As(V)]. The yield is studied with various parameters such as discharge current, duration of discharge and pH (2-10). The results are interpreted on the basis of interaction of the OH and eaq (produced consequent to the interaction of H2O+ and e with water at the surface of the solution) with arsenite [As(III)] through the intermediate oxidation state, namely [As(IV)].
基金The project partially supported by the Project of Key Science and Technology of Education Ministry (00250), the Natural ScienceFoundation of Gansu Province (3ZS041-A25-028), and the Project of KJCXGC-01, NWNU, China
文摘The oxidative degradation of 4-chlorophenol (4-CP) in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined by high performance liquid chromatography (HPLC). Various influencing factors such as the initial pH, the concentration of 4-CP and the catalytic action of Fe^2+ were examined. The results indicate that 4-CP is eventually degraded into inorganic ion, dioxide carbon and water. The attack of hydroxyl radicals on the benzene rings of 4-CP in the initial stage of oxidative reactions is presumed to be a key step. They also suggest that the reaction is of a pseudo-first order kinetic reaction and the proposed method is an efficient way for the 4-CP degradation,
基金support from "Open Research Center" Projects for Private Universities:matching fund subsidy from Ministry of Education,Culture,Sports,Science and Technology,2007-2011
文摘Exhaustive mineralization of pentachlorophenolate ion(PCP) in phosphate buffer was carried out using anodic contact glow discharge electrolysis(CGDE),in which plasma was sustained between the electrolyte and anode.During CGDE,PCP degraded smoothly.The amount of total organic carbon decreased significantly,indicating the eventual conversion of the carbon atoms of benzene nucleus to inorganic carbons.Furthermore,chlorine atoms in PCP were liberated as chloride ions.As a primary intermediate product,2,3,5,6tetrachloro-1,4-benzoquinone was detected,and oxalate and formate as byproducts were also found.It was revealed that disappearance of PCP obeyed first-order kinetics.The reaction rate was generally unaffected by both O2 and inert gases in the cell,although it decreased by raising initial pH of solution.In addition,a plausible reaction pathway involving hydroxyl radical was proposed.
基金supported by the 'Youth Science Foundation of University of Science and Technology Liaoning', 2012-2014
文摘Destruction of 4-phenolsulfonic acid (4-PSA) in water was carded out using anodic contact glow discharge electrolysis. Accompanying the decay of 4-PSA, the amount of total organic carbon (TOC) in water correspondingly decreased, while the sulfonate group of 4- PSA was released as sulfate ion. Oxalate and formate were obtained as minor by-products. Additionally, phenol, 1,4-hydroquinone, hydroxyquinol and 1,4-benzoquinone were detected as primary intermediates in the initial stages of decomposition of 4-PSA. A reaction pathway involving successive attacks of hydroxyl and hydrogen radicals was assumed on the basis of the observed products and kinetics. It was revealed that the decay of both 4-PSA and TOC obeyed a first-order rate law. The effects of different Fe ions and initial concentrations of 4-PSA on the degradation rate were investigated. It was found that the presence of Fe ions could increase the degradation rate of 4-PSA, while initial concentrations lower than 80 mmol/L had no significant effect on kinetic behaviour. The disappearance rate of 4-PSA was significantly affected by pH.
基金The project supported in part by the Project of Key Science and Technology of Education Ministry (00250)the Nature Science Foundation of Gansu Province (3ZS041-A25-028)the Invention Project of Science and Technology (KJCXGC-01, NWNU), 2000
文摘In an aqueous solution, normal electrolysis at high voltages switches over spontaneously to glow discharge electrolysis and gives rise to hydroxyl radical, hydrogen peroxide, and aqueous electron, as well as several other active species. Hydroxyl radical directly attacks organic contaminants to make them oxidized. In the present paper, 2-naphthylamine is eventually degraded into hydrogen carbonate and carbon dioxide. The degradation process is analyzed by using an Ultraviolet (UV) absorption spectrum, high-performance liquid chromatography (HPLC) and chemical oxygen demand (COD). It is demonstrated that 2-naphthylamine (co =30 mg·1-1) is completely converted within 2h at 30℃ and 600 V by glow discharge electrolysis, and the degradation is strongly dependent upon the presence of ferrous ions. COD is ascended in the absence of ferrous ions and descended in the presence of them.
基金The project supported by the Key Project of Science and Technology from the Ministry of Education China (No. 00250) the project of KJCXGC-01 of Northwest Normal University, China
文摘Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that the degradation followed the first order kinetic law; Fe2+ had a remarkable catalytic effect on the removal rate of o-chloropenol. In the presence of Fe2+, 2-CP underwent an exhaustive degradation, from which the major intermediates included o-dihydroxybenze, p-hydroxybenze, p-benzoquione and carboxlic acids.
基金Supported by the Key Development Program Foundation of Guangdong Province (No.2002C20809, 2004B50101001, 2005B50101001) Key Development Program Foundation of Guangxi Autonomy (No.0322012-8)
文摘The application and characteristics of relatively big volume plasma produced with cathodic glow discharges taking place across a gaseous envelope over the cathode which was dipped into electrolyte in hydrogen generation were studied. A critical investigation of the influence of methanol concentration and voltage across the circuit on the composition and power consumption per cubic meter of cathode liberating gas was carried out. The course of plasma under-liquid electrolysis has the typical characteristics of glow discharge electrolysis. The cathode liberating gas was in substantial excess of the Faraday law value. When the voltage across the circuit was equal to 550 V,the volume of cathodic gas with sodium carbonate solution was equal to 16.97 times the Faraday law value. The study showed that methanol molecules are more active than water molecules. The methanol molecules were decomposed at the plasma-catholyte interface by the radicals coming out the plasma mantle. Energy consumption per cubic meter of cathodic gases (WV) decreased while methanol concentration of the electrolytes increased. When methanol concentration equaled 5% (-),WV was 10.381×103 kJ/m3,less than the corresponding theoretic value of conventional water electrolysis method. The cathodic liberating gas was a mixture of hydrogen,carbon dioxide and carbon monoxide with over 95% hydrogen,if methanol concentration was more than 15% (-). The present research work revealed an innovative application of glow discharge and a new highly efficient hydrogen generation method,which depleted less resource and energy than normal electrolysis and is environmentally friendly.