The Ti-Supported MnO_2 electrode was modified by introducing SnO_2+RuO_2+MnO_2 as an intermediate layer into the Ti/MnO_2 interface. The anodic polarization curves were measured at various temperatures ranging from 30...The Ti-Supported MnO_2 electrode was modified by introducing SnO_2+RuO_2+MnO_2 as an intermediate layer into the Ti/MnO_2 interface. The anodic polarization curves were measured at various temperatures ranging from 30 to 80℃ and the activation energy for the oxygen evolution reaction was evaluated. The experimental activation energy increased linearly with increasing the overpotential. The activation energy at the equilibrium potential was linearly correlated with the difference between the crystal field stabilization energies of Mn^(4+) at initial state and Mn^(4+) at transition state. The electrocatalysis characteristics of the anode were discussed by means of the mechanism of the substitution reaction of the ligand(S_N1 and S_N2) and molecular orbital theory. The results show that the anode has better electrocatalystic characteristics.展开更多
The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electr...The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electrochemical perromance of the coke modified with various active components was studied. The results show that the coke modified with Fe（NO3）2 has the lowest energy consumption and higher COD removal rate under the same condition, and the modified coke has better surface characteristics for the purpose of this study. In addition, the kinetic constant was also calculated. The study shows that the three-dimensional electrode system with Fe （NO3）z-modified coke can give a satisfactory solution in biologically pretreated coking wastewater.展开更多
Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electroche...Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand（COD）analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions（0.2wt%NaCl）,and a three-dimensional（3D） reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline（200 mL of 100mg·L-（-1）） and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-（-2）,pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.展开更多
Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The p...Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The physicochemical properties of the Sb-SnO2 coating were markedly influenced by different amounts of Sb dopant. The electrodes, which contained 5% Sb dopant in the coating, presented a much more homogenous surface and much smaller mud-cracks, compared with Ti/Sb-SnO2 electrodes containing 10% or 15% Sb dopant, which exibited larger mud cracks and pores on the surface. However, the main microstructure remained unchanged with the addition of the Sb dopant. No new crystal phase was observed by X-ray diffraction （XRD）. The electrochemical oxidation of 4-chlorophenol on the Ti/SnO2 electrode with 5% Sb dopant was inclined to electrochemical combustion; while for those containing more Sb dopant, intermediate species were accumulated. The electrodes with 5% Sb dopant showed the highest efficiency in the bulk electrolysis of 4-chlorophenol at a current density of 20 mA/cm^2 for 180 min; and the removal rates of 4-chlorophenol and COD were 51.0% and 48.9%, respectively.展开更多
Ti3C2Tx,a novel two-dimensional layer material,is widely used as electrode materials of supercapacitor due to its good metal conductivity,redox reaction active surface,and so on.However,there are many challenges to be...Ti3C2Tx,a novel two-dimensional layer material,is widely used as electrode materials of supercapacitor due to its good metal conductivity,redox reaction active surface,and so on.However,there are many challenges to be addressed which impede Ti3C2Tx obtaining the ideal specific capacitance,such as restacking,re-crushing,and oxidation of titanium.Recently,many advances have been proposed to enhance capacitance performance of Ti3C2Tx.In this review,recent strategies for improving specific capacitance are summarized and compared,for example,film formation,surface modification,and composite method.Furthermore,in order to comprehend the mechanism of those efforts,this review analyzes the energy storage performance in different electrolytes and influencing factors.This review is expected to predict redouble research direction of Ti3C2Tx materials in supercapacitors.展开更多
Praseodymium was selected as a promoter for SnO2/Ti electrode to improve the electrocatalytic performance by electrodeposition in pharmaceutical wastewater treatment; the micrograph and the structure were characterize...Praseodymium was selected as a promoter for SnO2/Ti electrode to improve the electrocatalytic performance by electrodeposition in pharmaceutical wastewater treatment; the micrograph and the structure were characterized by SEM and XRD. Mixture uniform design was used in the optimization of the electrolytic conditions; mathematical model was established according to the rate of wiping COD off, which revealed the relationship between the current intensity, time of electrolysis, the amount of doped Pr, and the ratio of area （SnOJTi：Al）. On the basis of the analysis of the empirical model, the optimized parameters had been obtained; the rate of wiping COD off was up to 94.9%, it decreased from 392 to 20 mg/L. Experimental results showed that the electrocatalytic performance of the electrode doped with Pr was superior for the treatment of pharmaceutical wastewater.展开更多
Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH ...Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH （3-11） and initial concentration （5-200 mg/L）were evaluated. Thedegradation of2,4-DCP followed apparent pseudo first-order kinetics. Thedegradation ratio on Ti/SnO2 -Sb anode attained 〉 99.9% after 20 min of electrolysis at initial 5-200 mg/L concentrations at a constant currentdensity of 30 mA/cm2 with a 10 mmol/L sodium sulphate （Na2SO4 ） supporting electrolyte solution. The results showed that 2,4-DCP （100 mg/L）degradation and total organic carbon （TOC） removal ratio achieved 99.9% and 92.8%, respectively, at the optimal conditions after 30 min electrolysis. Under this condition, thedegradation rate constant （k） and thedegradation half-life （t1/2 ）were 0.21 min1 and （2.8 ± 0.2） min, respectively. Mainly carboxylic acids （propanoic acid, maleic acid, propanedioic acid, acetic acid and oxalic acid） weredetected as intermediates. The energy efficiencies for2,4-DCPdegradation （5-200 mg/L）with Ti/SnO2-Sb anode ranged from 0.672 to 1.602 g/kWh. The Ti/SnO2-Sb anodewith a high activity to rapid organic oxidation could be employed todegrade chlorophenols, particularly2,4-DCP inwastewater.展开更多
Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)como...Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)comodified Ti/PbO_(2)electrodes(Ti/PbO2CeSDBS).Ce and SDBS could greatly change the electronic structure and interface property of PbO2.Ti/PbO_(2)CeSDBS exhibited excellent electrocatalytic activity and stability in Rhodamine B(RhB)electrocatalytic oxidation reaction.The improved electrocatalytic activity associates with the synergistic effect of electronic and interface factors.In the electrochemical degradation of RhB,the removal efficiencies of RhB and COD are about 0.880 and 0.694 respectively after the electrolysis of 220 min with Ti/PbO_(2)Ce4SDBS40,which are higher than the contrast Ti/PbO_(2)electrodes.In the meantime,the accelerated lifetime of Ti/PbO_(2)Ce4SDBS40 is more than 6.2 times than that of Ti/PbO_(2).展开更多
Ti/SnO2–Sb electrode has a good effect on the removal of organic pollutants. But its short service life limits its large-scale application in industry. Electro-catalytic degradation performances and service life of t...Ti/SnO2–Sb electrode has a good effect on the removal of organic pollutants. But its short service life limits its large-scale application in industry. Electro-catalytic degradation performances and service life of the electrode can be significantly improved by doping rare earth（RE） ions into the oxide coating of Ti/SnO2–Sb electrode. Ti/SnO2–Sb electrodes doped with different RE elements（Ce, Dy, La, and Eu） were prepared by the thermal decomposition method at 550 ℃. Electro-catalytic degradation performances of electrodes doped with different RE elements were evaluated by linear sweep voltammetry（LSV） and Tafel curves. During the electrolysis,the conversion of p-nitrophenol was performed with these electrodes as anodes under galvanostatic control. The structures and morphologies of the surface coating of the electrodes were characterized by scanning electron microscope（SEM）. The results demonstrate that the electro-catalytic degradation performances of Ti/SnO2–Sb electrodes are improved to different levels by doping different RE ions. Improved Ti/SnO2–Sb electrodes by the introduction of different RE have higher oxygen evolution potential, better electro-catalysis ability, better coverage,and longer electrode life.展开更多
The degradation of ethinylestradiol (EE, an orally bio-active estrogen) in an aqueous-methanolic solution using a Ti/TiO2 thin-film electrode and UV radiation (a photoelectrocatalytic system) was evaluated. Hence, HPL...The degradation of ethinylestradiol (EE, an orally bio-active estrogen) in an aqueous-methanolic solution using a Ti/TiO2 thin-film electrode and UV radiation (a photoelectrocatalytic system) was evaluated. Hence, HPLC/UV analysis shows that EE (at 0.34 mmol) is totally consumed after 30 minutes of exposure to the photoelectrocatalytic system in the presence of Na2SO4 (0.1 mol·L-1) and with an applied bias potential of +1.0 V versus the Ag/AgCl reference electrode. Moreover, monitoring by direct infusion electrospray ionization mass spectrometry (ESI-MS) and SPME-GC/ MS (solid phase microextraction coupled with gas chromatography-mass spectrometry) reveals that apparently no degradation products are formed under these conditions. Hence, this study demonstrates that the photoelectrocatalytic system can be efficiently used to promote the complete degradation (and likely mineralization) of this hormone under these conditions.展开更多
基金Supported by the National Natural Science Foundation of China.
文摘The Ti-Supported MnO_2 electrode was modified by introducing SnO_2+RuO_2+MnO_2 as an intermediate layer into the Ti/MnO_2 interface. The anodic polarization curves were measured at various temperatures ranging from 30 to 80℃ and the activation energy for the oxygen evolution reaction was evaluated. The experimental activation energy increased linearly with increasing the overpotential. The activation energy at the equilibrium potential was linearly correlated with the difference between the crystal field stabilization energies of Mn^(4+) at initial state and Mn^(4+) at transition state. The electrocatalysis characteristics of the anode were discussed by means of the mechanism of the substitution reaction of the ligand(S_N1 and S_N2) and molecular orbital theory. The results show that the anode has better electrocatalystic characteristics.
文摘The electrochemical treatment of COD contained in biologically pretreated coking wastewater treated by a three-dimensional electrode system with modified coke as the particle electrode was investigated. And the electrochemical perromance of the coke modified with various active components was studied. The results show that the coke modified with Fe（NO3）2 has the lowest energy consumption and higher COD removal rate under the same condition, and the modified coke has better surface characteristics for the purpose of this study. In addition, the kinetic constant was also calculated. The study shows that the three-dimensional electrode system with Fe （NO3）z-modified coke can give a satisfactory solution in biologically pretreated coking wastewater.
基金supported by the National Natural Science Foundation of China(21507104)the Fundamental Research Funds for the Central Universities of China
文摘Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand（COD）analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions（0.2wt%NaCl）,and a three-dimensional（3D） reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline（200 mL of 100mg·L-（-1）） and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-（-2）,pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.
基金Project supported by the Institute of Environmental Engineering,Peking University and China Postdoctoral Science Foundation(No.2005037032)
文摘Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The physicochemical properties of the Sb-SnO2 coating were markedly influenced by different amounts of Sb dopant. The electrodes, which contained 5% Sb dopant in the coating, presented a much more homogenous surface and much smaller mud-cracks, compared with Ti/Sb-SnO2 electrodes containing 10% or 15% Sb dopant, which exibited larger mud cracks and pores on the surface. However, the main microstructure remained unchanged with the addition of the Sb dopant. No new crystal phase was observed by X-ray diffraction （XRD）. The electrochemical oxidation of 4-chlorophenol on the Ti/SnO2 electrode with 5% Sb dopant was inclined to electrochemical combustion; while for those containing more Sb dopant, intermediate species were accumulated. The electrodes with 5% Sb dopant showed the highest efficiency in the bulk electrolysis of 4-chlorophenol at a current density of 20 mA/cm^2 for 180 min; and the removal rates of 4-chlorophenol and COD were 51.0% and 48.9%, respectively.
基金National Natural Science Foundation of China with Grant No.21905304Natural Science Foundation of Shandong Province(No.ZR2019BEM031)the Fundamental Research Funds for the Central Universities(Nos.18CX02158A and 19CX05001A).
文摘Ti3C2Tx,a novel two-dimensional layer material,is widely used as electrode materials of supercapacitor due to its good metal conductivity,redox reaction active surface,and so on.However,there are many challenges to be addressed which impede Ti3C2Tx obtaining the ideal specific capacitance,such as restacking,re-crushing,and oxidation of titanium.Recently,many advances have been proposed to enhance capacitance performance of Ti3C2Tx.In this review,recent strategies for improving specific capacitance are summarized and compared,for example,film formation,surface modification,and composite method.Furthermore,in order to comprehend the mechanism of those efforts,this review analyzes the energy storage performance in different electrolytes and influencing factors.This review is expected to predict redouble research direction of Ti3C2Tx materials in supercapacitors.
基金the Fund of the Natural Science of Guangxi (0731015)
文摘Praseodymium was selected as a promoter for SnO2/Ti electrode to improve the electrocatalytic performance by electrodeposition in pharmaceutical wastewater treatment; the micrograph and the structure were characterized by SEM and XRD. Mixture uniform design was used in the optimization of the electrolytic conditions; mathematical model was established according to the rate of wiping COD off, which revealed the relationship between the current intensity, time of electrolysis, the amount of doped Pr, and the ratio of area （SnOJTi：Al）. On the basis of the analysis of the empirical model, the optimized parameters had been obtained; the rate of wiping COD off was up to 94.9%, it decreased from 392 to 20 mg/L. Experimental results showed that the electrocatalytic performance of the electrode doped with Pr was superior for the treatment of pharmaceutical wastewater.
基金supported by the National Science Foundation for Innovative Research Group of China(No.51121003)the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20110003110023)the special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control of China
文摘Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH （3-11） and initial concentration （5-200 mg/L）were evaluated. Thedegradation of2,4-DCP followed apparent pseudo first-order kinetics. Thedegradation ratio on Ti/SnO2 -Sb anode attained 〉 99.9% after 20 min of electrolysis at initial 5-200 mg/L concentrations at a constant currentdensity of 30 mA/cm2 with a 10 mmol/L sodium sulphate （Na2SO4 ） supporting electrolyte solution. The results showed that 2,4-DCP （100 mg/L）degradation and total organic carbon （TOC） removal ratio achieved 99.9% and 92.8%, respectively, at the optimal conditions after 30 min electrolysis. Under this condition, thedegradation rate constant （k） and thedegradation half-life （t1/2 ）were 0.21 min1 and （2.8 ± 0.2） min, respectively. Mainly carboxylic acids （propanoic acid, maleic acid, propanedioic acid, acetic acid and oxalic acid） weredetected as intermediates. The energy efficiencies for2,4-DCPdegradation （5-200 mg/L）with Ti/SnO2-Sb anode ranged from 0.672 to 1.602 g/kWh. The Ti/SnO2-Sb anodewith a high activity to rapid organic oxidation could be employed todegrade chlorophenols, particularly2,4-DCP inwastewater.
基金Thanks to the financial support from the Science and technology project of Shaanxi Province(2017ZDXM-GY-041).
文摘Regulation of the electronic structure and interface property becomes a major strategy in the preparation of electrocatalyst.This paper reports the synthesis of cerium(Ce)and sodium dodecyl benzene sulfonate(SDBS)comodified Ti/PbO_(2)electrodes(Ti/PbO2CeSDBS).Ce and SDBS could greatly change the electronic structure and interface property of PbO2.Ti/PbO_(2)CeSDBS exhibited excellent electrocatalytic activity and stability in Rhodamine B(RhB)electrocatalytic oxidation reaction.The improved electrocatalytic activity associates with the synergistic effect of electronic and interface factors.In the electrochemical degradation of RhB,the removal efficiencies of RhB and COD are about 0.880 and 0.694 respectively after the electrolysis of 220 min with Ti/PbO_(2)Ce4SDBS40,which are higher than the contrast Ti/PbO_(2)electrodes.In the meantime,the accelerated lifetime of Ti/PbO_(2)Ce4SDBS40 is more than 6.2 times than that of Ti/PbO_(2).
基金financially supported by the National Natural Science Foundation of China (No. 51364024 and 51404124)Gansu Province Department of Education Fund (No. 2013A-029)the Foundation of State Key Laboratory of Gansu Advanced Nonferrous Metal Materials (Nos. SKL 1316 and SKL 1314)
文摘Ti/SnO2–Sb electrode has a good effect on the removal of organic pollutants. But its short service life limits its large-scale application in industry. Electro-catalytic degradation performances and service life of the electrode can be significantly improved by doping rare earth（RE） ions into the oxide coating of Ti/SnO2–Sb electrode. Ti/SnO2–Sb electrodes doped with different RE elements（Ce, Dy, La, and Eu） were prepared by the thermal decomposition method at 550 ℃. Electro-catalytic degradation performances of electrodes doped with different RE elements were evaluated by linear sweep voltammetry（LSV） and Tafel curves. During the electrolysis,the conversion of p-nitrophenol was performed with these electrodes as anodes under galvanostatic control. The structures and morphologies of the surface coating of the electrodes were characterized by scanning electron microscope（SEM）. The results demonstrate that the electro-catalytic degradation performances of Ti/SnO2–Sb electrodes are improved to different levels by doping different RE ions. Improved Ti/SnO2–Sb electrodes by the introduction of different RE have higher oxygen evolution potential, better electro-catalysis ability, better coverage,and longer electrode life.
文摘采用溶胶-凝胶法制备高活性Ti基纳米TiO2-ZrO2膜电极.通过X射线衍射分析表明,纳米TiO2-ZrO2粉体呈微-纳二级结构.扫描电子显微镜测试表明,颗粒平均尺寸约为30 nm.通过循环伏安和恒电流电解技术研究发现,Ti/nanoTiO2-ZrO2电极对马来酸电催化还原制备丁二酸的活性要高于Ti/nanoTiO2电极,反应过程受扩散控制.以钛基氧化钌电极为阳极,Ti/nano TiO2-ZrO2膜电极为阴极进行恒电流电解实验.结果表明,控制电流密度20 mA cm-2,温度60℃,丁二酸的产率达到96%.
文摘The degradation of ethinylestradiol (EE, an orally bio-active estrogen) in an aqueous-methanolic solution using a Ti/TiO2 thin-film electrode and UV radiation (a photoelectrocatalytic system) was evaluated. Hence, HPLC/UV analysis shows that EE (at 0.34 mmol) is totally consumed after 30 minutes of exposure to the photoelectrocatalytic system in the presence of Na2SO4 (0.1 mol·L-1) and with an applied bias potential of +1.0 V versus the Ag/AgCl reference electrode. Moreover, monitoring by direct infusion electrospray ionization mass spectrometry (ESI-MS) and SPME-GC/ MS (solid phase microextraction coupled with gas chromatography-mass spectrometry) reveals that apparently no degradation products are formed under these conditions. Hence, this study demonstrates that the photoelectrocatalytic system can be efficiently used to promote the complete degradation (and likely mineralization) of this hormone under these conditions.
