The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towa...The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towards methanol electro-oxidation was evaluated by cyclic voltammetry in 1 mol/L KOH solution.XRD and TEM analyses revealed that nano-decomposition of quasicrystal grains occurred in the initial stage of dealloying,and the fully dealloyed sample was composed of FCC-Pd phase.Scanning electron microscopy observation indicated that a maze-like nanoporous pattern was formed in the dealloyed sample,consisting of percolated pores of 5.20 nm in diameter in a skeleton of randomly-orientated Pd nano-ligaments with a uniform thickness of^5 nm.A retention of^12 at.%Al in the Pd nano-ligments was determined by energy dispersive X-ray spectroscopy(EDS).The nanoporous Pd demonstrated obvious electro-catalytic activity towards methanol electro-oxidation in alkaline environment.展开更多
The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nan...The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nanopowder modified electrode was prepared using the drop coating method,which displayed excellent electrocatalytic activity towards the oxidation of dopamine and uric acid compared with the bare glassy carbon electrode in phosphate buffer solution at pH=7.0.Linear responses for dopamine and uric acid were obtained in the ranges of3.3μmol/L to 249.1μmol/L and 6.7μmol/L to 386.3μmol/L with detection limits of 1.5μmol/L and 2.7μmol/L(S/N=3),respectively.The response time was less than 2 s in case of dopamine and 3 s in case of uric acid,respectively.The results demonstrated that the graphene nanopowder had potential for detecting dopamine and uric acid.展开更多
Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope(SEM), X-ray diffraction(XRD) and cyclic voltammetry...Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope(SEM), X-ray diffraction(XRD) and cyclic voltammetry(CV) measurements. The electro-catalytic activity for degradation of sulfisoxazole(SIZ) was investigated by using prepared graphene or graphite anode. The results showed that the degradation of SIZ was much more rapid on the graphene than that on the graphite electrode. Moreover, the graphene electrode exhibited good stability and recyclability. The analysis on the intermediate products and the measurement of active species during the SIZ degradation demonstrated that indirect oxidation is the dominant mechanism, involving the electro-catalytic generation of OH and O_2^- as the main active oxygen species. This study implies that graphene is a promising potential electrode material for long-term application to electro-catalytic degradation of organic pollutants.展开更多
The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode...The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.展开更多
Lithium-sulfur(Li-S)batteries with high energy densities have received increasing attention.However,the electrochemical performance of Li-S batteries is still far from the satisfactory of the practical application,whi...Lithium-sulfur(Li-S)batteries with high energy densities have received increasing attention.However,the electrochemical performance of Li-S batteries is still far from the satisfactory of the practical application,which can be mainly attributed to the shuttling of polysulfides and the slow reaction kinetics of polysulfide conversion.To address this issue,a 3D porous carbon structure constructed by 2D N-doped graphene and 1D carbon nanotubes with embedded Fe3C/Fe nanoparticles(NG@Fe3C/Fe)was designed and prepared by a simple programmed calcination method for the modification of polypropylene(PP)separator.The Fe3C/Fe nanoparticles demonstrate an excellent catalytic conversion and strong chemisorption towards polysulfides,while the unique architecture of N-doped graphene promotes the Li+/electron transfer and the physical adsorption of polysulfides.The electrochemical performance of the Li-S batteries with the NG@Fe3C/Fe-modified separator is significantly improved.A large discharge capacity of 1481 mA∙h∙g-1 is achieved at 0.2 C(1 C=1675 mA/g),and a high capacity of 601 mA∙h∙g-1 is maintained after discharged/charged for 500 cycles at a current rate of 1 C.This work provides a new approach for the development of high-performance Li-S batteries through the modification of the PP separator by rationally designed composites with large adsorption capability to polysulfides,good wettability to the electrolyte and high catalytic property.展开更多
Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxi...Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxidation of hydrazine and that involved in the rate-determining step were four and one,respectively.The interfering effect of some cations,anions and organic compounds were examined.Peak current for this process varied linearly with the square root of the scan rate.The kinetic parameters,such as the electron transfer coefficient(α) and catalytic rate constant(k) ,were determined using cyclic voltammetry,linear sweep voltammetry and chronoamperometry.The electro-catalytic response was optimized with regards to the pH,scan rate,hydrazine concentration and other variables.展开更多
The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging prob...The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging problems. In this paper, Electrocatalytically active palladium nanoparticles(Pd NPs) on MWNTs with the high-performance and excellent solubility polymer, poly(dimethylbenzimidazolium) iodide(P(DMBI)-I-)as modifier and glue was first discussed. The results of transmission electron microscopy(TEM) demonstrate a better dispersion of MWNTs with the assist of P(DMBI)-I-. The Raman spectra indicate a strong π-π interaction between MWNTs and P(DMBI)-I-. Taking advantages of the coordination effect of imidazole groups and the electrostatic attraction to Pd NPs, the prepared Pd/MWNTs-P(DMBI)-I-(Pd/MPDI-) hybrid is of well electrocatalytic activity to the ethanol fuel cells by electrochemical measurements. So it is believed that P(DMBI)-Ican be further applied in the dispersion of different carbon-based materials and metal nanoparticles for fabricating more novel composites for catalyst and electrode material.展开更多
基金Foundation item:Project(51671045)supported by the National Natural Science Foundation of ChinaProject(DUT18GF112)supported by the Fundamental Research Funds for the Central Universities,ChinaProject(TZ2016004)supported by the Science Challenge Project,China
文摘The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towards methanol electro-oxidation was evaluated by cyclic voltammetry in 1 mol/L KOH solution.XRD and TEM analyses revealed that nano-decomposition of quasicrystal grains occurred in the initial stage of dealloying,and the fully dealloyed sample was composed of FCC-Pd phase.Scanning electron microscopy observation indicated that a maze-like nanoporous pattern was formed in the dealloyed sample,consisting of percolated pores of 5.20 nm in diameter in a skeleton of randomly-orientated Pd nano-ligaments with a uniform thickness of^5 nm.A retention of^12 at.%Al in the Pd nano-ligments was determined by energy dispersive X-ray spectroscopy(EDS).The nanoporous Pd demonstrated obvious electro-catalytic activity towards methanol electro-oxidation in alkaline environment.
基金supported by the National Natural Science Foundation(11179033)Beijing Natural Science Foundation(2102012)
文摘The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nanopowder modified electrode was prepared using the drop coating method,which displayed excellent electrocatalytic activity towards the oxidation of dopamine and uric acid compared with the bare glassy carbon electrode in phosphate buffer solution at pH=7.0.Linear responses for dopamine and uric acid were obtained in the ranges of3.3μmol/L to 249.1μmol/L and 6.7μmol/L to 386.3μmol/L with detection limits of 1.5μmol/L and 2.7μmol/L(S/N=3),respectively.The response time was less than 2 s in case of dopamine and 3 s in case of uric acid,respectively.The results demonstrated that the graphene nanopowder had potential for detecting dopamine and uric acid.
基金supported by the National Natural Science Foundation of China (Nos. 21377067, 21407092, 21177072)the Master's Degree Thesis Excellent Training Fund of Three Gorges University (No. 2014PY074)
文摘Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope(SEM), X-ray diffraction(XRD) and cyclic voltammetry(CV) measurements. The electro-catalytic activity for degradation of sulfisoxazole(SIZ) was investigated by using prepared graphene or graphite anode. The results showed that the degradation of SIZ was much more rapid on the graphene than that on the graphite electrode. Moreover, the graphene electrode exhibited good stability and recyclability. The analysis on the intermediate products and the measurement of active species during the SIZ degradation demonstrated that indirect oxidation is the dominant mechanism, involving the electro-catalytic generation of OH and O_2^- as the main active oxygen species. This study implies that graphene is a promising potential electrode material for long-term application to electro-catalytic degradation of organic pollutants.
基金Project(50925417)supported by the National Natureal Science Foundation for Distinguished Young Scholar of ChinaProject(51074191)supported by the National Natural Science Foundation of China
文摘The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.
基金This work was supported by the National Natural Science Foundation of China (Nos.21931005,21871177,20172012002)the Natural Science Foundation of Shanghai,China(No.20ZR1427600)the Project of the Shanghai Science and Technology Committee,China(No.19JC1412600).
文摘Lithium-sulfur(Li-S)batteries with high energy densities have received increasing attention.However,the electrochemical performance of Li-S batteries is still far from the satisfactory of the practical application,which can be mainly attributed to the shuttling of polysulfides and the slow reaction kinetics of polysulfide conversion.To address this issue,a 3D porous carbon structure constructed by 2D N-doped graphene and 1D carbon nanotubes with embedded Fe3C/Fe nanoparticles(NG@Fe3C/Fe)was designed and prepared by a simple programmed calcination method for the modification of polypropylene(PP)separator.The Fe3C/Fe nanoparticles demonstrate an excellent catalytic conversion and strong chemisorption towards polysulfides,while the unique architecture of N-doped graphene promotes the Li+/electron transfer and the physical adsorption of polysulfides.The electrochemical performance of the Li-S batteries with the NG@Fe3C/Fe-modified separator is significantly improved.A large discharge capacity of 1481 mA∙h∙g-1 is achieved at 0.2 C(1 C=1675 mA/g),and a high capacity of 601 mA∙h∙g-1 is maintained after discharged/charged for 500 cycles at a current rate of 1 C.This work provides a new approach for the development of high-performance Li-S batteries through the modification of the PP separator by rationally designed composites with large adsorption capability to polysulfides,good wettability to the electrolyte and high catalytic property.
文摘Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxidation of hydrazine and that involved in the rate-determining step were four and one,respectively.The interfering effect of some cations,anions and organic compounds were examined.Peak current for this process varied linearly with the square root of the scan rate.The kinetic parameters,such as the electron transfer coefficient(α) and catalytic rate constant(k) ,were determined using cyclic voltammetry,linear sweep voltammetry and chronoamperometry.The electro-catalytic response was optimized with regards to the pH,scan rate,hydrazine concentration and other variables.
文摘The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging problems. In this paper, Electrocatalytically active palladium nanoparticles(Pd NPs) on MWNTs with the high-performance and excellent solubility polymer, poly(dimethylbenzimidazolium) iodide(P(DMBI)-I-)as modifier and glue was first discussed. The results of transmission electron microscopy(TEM) demonstrate a better dispersion of MWNTs with the assist of P(DMBI)-I-. The Raman spectra indicate a strong π-π interaction between MWNTs and P(DMBI)-I-. Taking advantages of the coordination effect of imidazole groups and the electrostatic attraction to Pd NPs, the prepared Pd/MWNTs-P(DMBI)-I-(Pd/MPDI-) hybrid is of well electrocatalytic activity to the ethanol fuel cells by electrochemical measurements. So it is believed that P(DMBI)-Ican be further applied in the dispersion of different carbon-based materials and metal nanoparticles for fabricating more novel composites for catalyst and electrode material.