The α-PbO2 electrodes are prepared by anodic electrodeposition on Al/conductive coating electrode from alkaline plumbite solutions in order to investigate the effect of the different current densities on the properti...The α-PbO2 electrodes are prepared by anodic electrodeposition on Al/conductive coating electrode from alkaline plumbite solutions in order to investigate the effect of the different current densities on the properties of α-PbO2 electrodes. The physic- ochemical properties of the α-PbO2 electrodes are analyzed by using SEM, EDS, XRD, Tafel plot, linear sweep voltammetry (LSV) and A.C. impedance. A compact and uniform layer of lead dioxide :)vas obtained at the current density of 3 mA.cm-2. A further increase in current density results in smaller particles with high porosity. EDS and XRD analyses have shown that the PbO2 deposited in alkaline conditions is highly non stoichiometric, and the PbO impurities are formed on the surface layer besides the α-PbO2. The corrosion resistance of α-PbO2 at the low current density is superior to that of the high current density. It can be attributed to a porous layer of deposited films at high current densities in aqueous Zn2+ 50 g·L^-1, H2SO4 150 When used as anodes for oxygen evolution g·L^-1, the Al/conductive coating/α-PbO2 exhibits lower potential compared to Pb electrode. Al/conductive coating/α-PbO2 electrode with the best electrocatalytic activity was obtained at current density of 1 mA·cm^-2. The lowest roughnest factor was obtained at 1 mA·cm^-2.展开更多
Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared ...Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared with that at the electrodes mingled with Bi or La prepared by electro-deposition. The experimental results indicate that the highest concentration of hydroxyl radicals generated by thermal-deposition, electro-deposition mingled with nothing, electro-deposition mingled with Bi or La was 0.781, 1.048, 1.838 or 2.044 μmol/L, respectively. When phenol was electrolyzed on the four electrodes at a current density of 30 mA/cm2, the removal efficiency of phenol after electrolysis for 1.5 h was 87.30%, 93.55%, 97.95% or 98.70%, TOC removal efficiency after electrolysis for 5 h was 86.76%, 94.26%, 98.53% or 99.60%, respectively. Through the degradation experiments of phenol, the amount of hydroxyl radicals was responsible for the removal efficiency of phenol. The electro-catalytic characteristics were investigated by SEM, the generation amount of hydroxyl radicals, the degradation degree of phenol and the stability and conductivity of the electrodes were also investigated. The experimental results indicate that the four electrodes all show good electro-catalytic characteristics; the electro-catalytic characteristics of the electrode mingled with La were superior to those of the other three ones, and the electrochemical degradation of phenol followed one-step reaction dynamics.展开更多
Iodinated trihalomethanes(I-THMs)in drinking water pipelines have attracted wide attention due to their high toxicity.The coexistence of widely present lead dioxide(PbO_(2))with commonly used disinfectant sodium hypoc...Iodinated trihalomethanes(I-THMs)in drinking water pipelines have attracted wide attention due to their high toxicity.The coexistence of widely present lead dioxide(PbO_(2))with commonly used disinfectant sodium hypochlorite(NaClO)in drinking water might change the formation characteristics of I-THMs due to the strongly oxidizing properties of PbO_(2).This study investigated the formation of I-THMs during the co-oxidation of natural organic matter including humic acid(HA),extracellular organic matter(EOM),and intracellular organic matter(IOM)of algogenic organic matter by PbO_(2) and NaClO.Triiodomethane(CHI_(3))is the dominant product in the single oxidation system of PbO_(2),whereas trichloromethane(CHCl_(3)),chlorodiiodomethane(CHClI_(2)),and dichloroiodomethane(CHCl2I)are the major products in the single NaClO system.In the co-oxidation system,the dominant I-THMs are similar to those in the single NaClO system.However,the CHCl_(3) content decreased to 56.4%whereas I-THMs concentrations remained unchanged with the increase of PbO_(2) concentration.The main reason is attributed to the reduced residual chlorine content due to the reaction of PbO_(2) with NaClO.IOM is more prone to forming I-THMs than HA and EOM due to the specified structures.This study suggested that PbO_(2) in the drinking water supply pipelines might change the risk of THMs.展开更多
The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide(F--PbO2) electrode for ...The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide(F--PbO2) electrode for the degradation of aniline was compared with that of undoped lead dioxide(PbO2) electrode by ultraviolet-visible(UV-Vis) spectroscopy,linear voltammetry and other analytical methods,such as the measurement by chemical oxygen demand analyzer,high performance liquid chromatography and scanning electron micrography.It was shown that both PbO2 electrode and F--PbO2 electrode could make aniline be mineralized completely and have the same degradation course,but F--PbO2 electrode has much higher electrocatalytic activity than undoped PbO2 electrode for the electrochemical degradation of aniline.The experimental results confirm that F--PbO2 electrode has much higher potential for oxygen evolution than undoped PbO2 electrode.展开更多
The kinetics of oxygen evolution reaction(OER)on PbO_2-Ti/MnO_2 electrode has been studied using galvanistatic technique.In terms of kinetic parameters,the reaction path of OER is proposed.The electrocataIytic activit...The kinetics of oxygen evolution reaction(OER)on PbO_2-Ti/MnO_2 electrode has been studied using galvanistatic technique.In terms of kinetic parameters,the reaction path of OER is proposed.The electrocataIytic activity of lead dioxide and manganese dioxide has been discussed according to the theory of molecular orbit and quantum chemistry caIculation.It is concluded that the electrocatalytic activity of manganese dioxide is higher than that of lead dioxid,which is in agreement with the experimental result.展开更多
Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepare...Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepared for electrocatalytically oxidizing gaseous toluene in an all-solid cell at ambient temperature.The complex Ti/Sb-Sn O_(2)/β-Pb O_(2)anode,which was prepared by sequentially deposing Sb-Sn O_(2)and β-Pb O_(2)on a foam Ti substrate,shows high electrocatalytic oxidation efficiency of toluene (80%) at 7 hr of reaction and high CO_(2)selectivity (94.9%) under an optimized condition,i.e.,a cell voltage of 2.0 V,relative humidity of60%and a flow rate of 100 m L/min.The better catalytic performance can be ascribed to the high production rate of·OH radicals from discharging adsorbed water and the inhibition of oxygen evolution on the surface of foam Ti/Sb-Sn O_(2)/β-Pb O_(2)anode when compared with the foam Ti/Sb-Sn O_(2)anode.Our results demonstrate that prepared complex electrodes can be potentially used for electrocatalytic removal of gaseous toluene at room temperature with a good performance.展开更多
Anodic oxidation electrodeposition is the primary way to prepare lead dioxide anode. The regulation of the external circuit for the reaction is a unique advantage of electrocatalytic reaction, which can regulate cryst...Anodic oxidation electrodeposition is the primary way to prepare lead dioxide anode. The regulation of the external circuit for the reaction is a unique advantage of electrocatalytic reaction, which can regulate crystallization and accelerate the reaction process. In this study, lead dioxide coatings with uniform pore size distribution were quickly prepared on three different substrates by potential linear increase electrodeposition(PLIED). Morphology and structure analysis shows that the prepared electrodes have uniform porous morphology, and Ti/SnO_(2)/PLIED has the smallest grain size. Three electrodes all display well degradation performance to azophloxine and diclofenac sodium. Ti/PLIED, and Ti/SnO_(2)/PLIED are appreciated for degrading organics with a simple structure in low concentrations. At the same time,Ti/SnO_(2)/PLIED is more suitable for complex organics in high concentrations. Electrochemical activity tests indicate the different mechanisms of the PLIED electrodes that build the other degradation performance.Three PLIED electrodes show excellent electrical and electrochemical stability during the cycle degradation process. The results provide a reference for the subsequent anodic oxidation electrodeposition research and the regulating effect of the external circuit on coating properties.展开更多
PbO_2/activated carbon(AC) hybrid supercapacitor in H_2SO_4 with a carbon foam current collector is studied.The PbO_2/AC hybrid is designed with electrodeposited PbO_2 thin film as positive electrode to match with A...PbO_2/activated carbon(AC) hybrid supercapacitor in H_2SO_4 with a carbon foam current collector is studied.The PbO_2/AC hybrid is designed with electrodeposited PbO_2 thin film as positive electrode to match with AC negative electrode.The discharge curve shows capacitive characteristics between 1.88 V and 0.65 V.The hybrid system exhibits excellent energy and power performance,with specific energy of 43.6 Wh/kg at a power density of 654.2 W/kg.The use of carbon foam current collector ensures stability of the PbO_2 electrode in H_2SO_4 environment.After 2600 deep cycles at 15 C high rate of charge/discharge,the capacity remains nearly unchanged from its initial value.展开更多
Despite of the hazardous risk of Pb^(2+) leakage, lead dioxide has been attributed as a quasi-ideal anode material with high oxygen evolution potential, excellent conductivity, good stability and low cost in electroch...Despite of the hazardous risk of Pb^(2+) leakage, lead dioxide has been attributed as a quasi-ideal anode material with high oxygen evolution potential, excellent conductivity, good stability and low cost in electrochemical oxidation wastewater treatment technique. In this study, a novel Ti/PbO_(2) anode was fabricated by embedding raw materials that are readily and cheaply available, i.e., hairs. The structure-activity relationship of the new electrode was firstly revealed by material and electrochemical characterizations. Then different levels of pollutants (azo dye, phenol and maleic acid) were used to investigate the electrochemical oxidation performance of the new electrode. Finally, the accelerated electrode lifetime and Pb^(2+) leakage tests were carried out. Results showed that the embedded hairs changed the preferential crystallographic orientation of PbO_(2) and decreased the grain size. Hairs introduced additional roughness and active sites, and decreased the electrode impedance, especially under 5 mg/cm^(2) of embedding amount. The removal efficiencies of different target pollutants were enhanced more or less by embedding appropriate amount of hairs, depending on the current density, but loading excessive hairs had a negative effect. The accumulation of intermediate products during phenol degradation was also changed by the hairs. The new electrode could undergo ~550 h of harsh electrolysis. It is also relieved that the Pb^(2+) leakage was found to be suppressed during this long-term electrolysis process.展开更多
基金supported by the Author of National Excellent Doctoral Dissertation of China (No.20050053)Analysis and Measurement Research Fund(2007-21) of Kunming University of Science and Technology
文摘The α-PbO2 electrodes are prepared by anodic electrodeposition on Al/conductive coating electrode from alkaline plumbite solutions in order to investigate the effect of the different current densities on the properties of α-PbO2 electrodes. The physic- ochemical properties of the α-PbO2 electrodes are analyzed by using SEM, EDS, XRD, Tafel plot, linear sweep voltammetry (LSV) and A.C. impedance. A compact and uniform layer of lead dioxide :)vas obtained at the current density of 3 mA.cm-2. A further increase in current density results in smaller particles with high porosity. EDS and XRD analyses have shown that the PbO2 deposited in alkaline conditions is highly non stoichiometric, and the PbO impurities are formed on the surface layer besides the α-PbO2. The corrosion resistance of α-PbO2 at the low current density is superior to that of the high current density. It can be attributed to a porous layer of deposited films at high current densities in aqueous Zn2+ 50 g·L^-1, H2SO4 150 When used as anodes for oxygen evolution g·L^-1, the Al/conductive coating/α-PbO2 exhibits lower potential compared to Pb electrode. Al/conductive coating/α-PbO2 electrode with the best electrocatalytic activity was obtained at current density of 1 mA·cm^-2. The lowest roughnest factor was obtained at 1 mA·cm^-2.
基金the Environment Bureau of Jilin Province, China(No.2006-11)Scientific Institute of Changchun City(No. 2007KZ15)985 Project of Jilin University
文摘Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared with that at the electrodes mingled with Bi or La prepared by electro-deposition. The experimental results indicate that the highest concentration of hydroxyl radicals generated by thermal-deposition, electro-deposition mingled with nothing, electro-deposition mingled with Bi or La was 0.781, 1.048, 1.838 or 2.044 μmol/L, respectively. When phenol was electrolyzed on the four electrodes at a current density of 30 mA/cm2, the removal efficiency of phenol after electrolysis for 1.5 h was 87.30%, 93.55%, 97.95% or 98.70%, TOC removal efficiency after electrolysis for 5 h was 86.76%, 94.26%, 98.53% or 99.60%, respectively. Through the degradation experiments of phenol, the amount of hydroxyl radicals was responsible for the removal efficiency of phenol. The electro-catalytic characteristics were investigated by SEM, the generation amount of hydroxyl radicals, the degradation degree of phenol and the stability and conductivity of the electrodes were also investigated. The experimental results indicate that the four electrodes all show good electro-catalytic characteristics; the electro-catalytic characteristics of the electrode mingled with La were superior to those of the other three ones, and the electrochemical degradation of phenol followed one-step reaction dynamics.
基金supported by the National Natural Science Foundation of China(No.22076141)the Fundamental Research Funds for the Central Universities,China(No.2022-4-YB-13).
文摘Iodinated trihalomethanes(I-THMs)in drinking water pipelines have attracted wide attention due to their high toxicity.The coexistence of widely present lead dioxide(PbO_(2))with commonly used disinfectant sodium hypochlorite(NaClO)in drinking water might change the formation characteristics of I-THMs due to the strongly oxidizing properties of PbO_(2).This study investigated the formation of I-THMs during the co-oxidation of natural organic matter including humic acid(HA),extracellular organic matter(EOM),and intracellular organic matter(IOM)of algogenic organic matter by PbO_(2) and NaClO.Triiodomethane(CHI_(3))is the dominant product in the single oxidation system of PbO_(2),whereas trichloromethane(CHCl_(3)),chlorodiiodomethane(CHClI_(2)),and dichloroiodomethane(CHCl2I)are the major products in the single NaClO system.In the co-oxidation system,the dominant I-THMs are similar to those in the single NaClO system.However,the CHCl_(3) content decreased to 56.4%whereas I-THMs concentrations remained unchanged with the increase of PbO_(2) concentration.The main reason is attributed to the reduced residual chlorine content due to the reaction of PbO_(2) with NaClO.IOM is more prone to forming I-THMs than HA and EOM due to the specified structures.This study suggested that PbO_(2) in the drinking water supply pipelines might change the risk of THMs.
基金Supported by the National Natural Science Foundation of China(No.20873051)the High-tech Research and Development Program of China(No.2006AA06Z321)the Natural Science Foundation of Jiangsu Province,China(No.BK2008555)
文摘The paper deals with the influence of anode material on the efficiency of degradation for organic pollutants in water system.The electrochemical performance of fluorine ion doped lead dioxide(F--PbO2) electrode for the degradation of aniline was compared with that of undoped lead dioxide(PbO2) electrode by ultraviolet-visible(UV-Vis) spectroscopy,linear voltammetry and other analytical methods,such as the measurement by chemical oxygen demand analyzer,high performance liquid chromatography and scanning electron micrography.It was shown that both PbO2 electrode and F--PbO2 electrode could make aniline be mineralized completely and have the same degradation course,but F--PbO2 electrode has much higher electrocatalytic activity than undoped PbO2 electrode for the electrochemical degradation of aniline.The experimental results confirm that F--PbO2 electrode has much higher potential for oxygen evolution than undoped PbO2 electrode.
文摘The kinetics of oxygen evolution reaction(OER)on PbO_2-Ti/MnO_2 electrode has been studied using galvanistatic technique.In terms of kinetic parameters,the reaction path of OER is proposed.The electrocataIytic activity of lead dioxide and manganese dioxide has been discussed according to the theory of molecular orbit and quantum chemistry caIculation.It is concluded that the electrocatalytic activity of manganese dioxide is higher than that of lead dioxid,which is in agreement with the experimental result.
基金supported by the National Natural Science Foundation of China (Nos. 22025604, 21976196, and 41877306)the Hebei Technological Innovation Center for Volatile Organic Compounds Detection and Treatment in Chemical Industry (No. ZXJJ20210403)。
文摘Mineralization of benzene,toluene,and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air.In this work,a foam Ti/Sb-Sn O2/β-Pb O_(2)anode catalyst was prepared for electrocatalytically oxidizing gaseous toluene in an all-solid cell at ambient temperature.The complex Ti/Sb-Sn O_(2)/β-Pb O_(2)anode,which was prepared by sequentially deposing Sb-Sn O_(2)and β-Pb O_(2)on a foam Ti substrate,shows high electrocatalytic oxidation efficiency of toluene (80%) at 7 hr of reaction and high CO_(2)selectivity (94.9%) under an optimized condition,i.e.,a cell voltage of 2.0 V,relative humidity of60%and a flow rate of 100 m L/min.The better catalytic performance can be ascribed to the high production rate of·OH radicals from discharging adsorbed water and the inhibition of oxygen evolution on the surface of foam Ti/Sb-Sn O_(2)/β-Pb O_(2)anode when compared with the foam Ti/Sb-Sn O_(2)anode.Our results demonstrate that prepared complex electrodes can be potentially used for electrocatalytic removal of gaseous toluene at room temperature with a good performance.
基金the financial supports from the National Natural Science Foundation of China (No. 52270078)the Natural Science Basic Research Plan in Shaanxi Province of China (No. 2021JM-012)+1 种基金the Welfare Technology Research Plan of Zhejiang Province (No. LZY21E080003)the Fundamental Research Funds for the Central Universities (No. xjh012020037)。
文摘Anodic oxidation electrodeposition is the primary way to prepare lead dioxide anode. The regulation of the external circuit for the reaction is a unique advantage of electrocatalytic reaction, which can regulate crystallization and accelerate the reaction process. In this study, lead dioxide coatings with uniform pore size distribution were quickly prepared on three different substrates by potential linear increase electrodeposition(PLIED). Morphology and structure analysis shows that the prepared electrodes have uniform porous morphology, and Ti/SnO_(2)/PLIED has the smallest grain size. Three electrodes all display well degradation performance to azophloxine and diclofenac sodium. Ti/PLIED, and Ti/SnO_(2)/PLIED are appreciated for degrading organics with a simple structure in low concentrations. At the same time,Ti/SnO_(2)/PLIED is more suitable for complex organics in high concentrations. Electrochemical activity tests indicate the different mechanisms of the PLIED electrodes that build the other degradation performance.Three PLIED electrodes show excellent electrical and electrochemical stability during the cycle degradation process. The results provide a reference for the subsequent anodic oxidation electrodeposition research and the regulating effect of the external circuit on coating properties.
基金the financial support of this research work from Natural Science Foundation of China(No 20663005)
文摘PbO_2/activated carbon(AC) hybrid supercapacitor in H_2SO_4 with a carbon foam current collector is studied.The PbO_2/AC hybrid is designed with electrodeposited PbO_2 thin film as positive electrode to match with AC negative electrode.The discharge curve shows capacitive characteristics between 1.88 V and 0.65 V.The hybrid system exhibits excellent energy and power performance,with specific energy of 43.6 Wh/kg at a power density of 654.2 W/kg.The use of carbon foam current collector ensures stability of the PbO_2 electrode in H_2SO_4 environment.After 2600 deep cycles at 15 C high rate of charge/discharge,the capacity remains nearly unchanged from its initial value.
基金financed by the National Natural Science Foundation of China (No. 21706153)Natural Science Basic Research Plan in Shaanxi Province of China (No. 2018JQ2066)。
文摘Despite of the hazardous risk of Pb^(2+) leakage, lead dioxide has been attributed as a quasi-ideal anode material with high oxygen evolution potential, excellent conductivity, good stability and low cost in electrochemical oxidation wastewater treatment technique. In this study, a novel Ti/PbO_(2) anode was fabricated by embedding raw materials that are readily and cheaply available, i.e., hairs. The structure-activity relationship of the new electrode was firstly revealed by material and electrochemical characterizations. Then different levels of pollutants (azo dye, phenol and maleic acid) were used to investigate the electrochemical oxidation performance of the new electrode. Finally, the accelerated electrode lifetime and Pb^(2+) leakage tests were carried out. Results showed that the embedded hairs changed the preferential crystallographic orientation of PbO_(2) and decreased the grain size. Hairs introduced additional roughness and active sites, and decreased the electrode impedance, especially under 5 mg/cm^(2) of embedding amount. The removal efficiencies of different target pollutants were enhanced more or less by embedding appropriate amount of hairs, depending on the current density, but loading excessive hairs had a negative effect. The accumulation of intermediate products during phenol degradation was also changed by the hairs. The new electrode could undergo ~550 h of harsh electrolysis. It is also relieved that the Pb^(2+) leakage was found to be suppressed during this long-term electrolysis process.