The temperature dependence of hydrogen evolution reaction （HER） at a quasi-single crystalline gold electrode in both 0.1 mol/L HCl04 and 0.1 mol/L KOH solutions was investigated by cyclic voltammetry. HER current di...The temperature dependence of hydrogen evolution reaction （HER） at a quasi-single crystalline gold electrode in both 0.1 mol/L HCl04 and 0.1 mol/L KOH solutions was investigated by cyclic voltammetry. HER current displays a clear increase with reaction overpotential （η） and temperature from 278-333 K. In 0.1 mol/L HClO4 the Tafel slopes are found to increases slightly with temperature from 118 mV/dec to 146 mV/dec, while in 0.1 mol/L KOH it is ca. 153±15 mV/dec without clear temperature-dependent trend. The apparent activation energy （Ea） for HER at equilibrium potential is ca. 48 and 34 kJ/mol in 0.1 mol/L HC104 and 0.1 mol/L KOH, respectively. In acid solution, Ea decreases with increase in η, from Ea-37 kJ/mol （η=0.2 V） to 30 kJ/mol （η=0.35 V）. In contrast, in 0.1 mol/L KOH, Ea does not show obvious change with U. The pre-exponential factor （A） in 0.1 mol/L HC104 is ca. 1 order higher than that in 0.1 mol/L KOH. Toward more negative potential, in 0.1 mol/L HC104 A changes little with potential, while in 0.1 mol/L KOH it displays a monotonic increase with U. The change trends of the potential-dependent kinetic parameters for HER at Au electrode in 0.1 mol/L HClO4 and that in 0.1 mol/L KOH are discussed.展开更多
The hydrogen peroxide oxidation reaction (HPOOR) on Au(111) electrode in alkaline solutions with pH values ranging from 10 to 13 was examined systematically. HPOOR activity increased and the slope of the i-E curve dec...The hydrogen peroxide oxidation reaction (HPOOR) on Au(111) electrode in alkaline solutions with pH values ranging from 10 to 13 was examined systematically. HPOOR activity increased and the slope of the i-E curve decreased with increasing pH. HO2- is suggested to be the main reactive intermediate for HPOOR in alkaline media. The fast kinetics for HPOOR in alkaline solution is facilitated by the electrostatic interaction between the positively charged electrode and the reactive anions (i.e., HO2- and HO-), which increases the concentration of these reactants and the thermodynamic driving force for HO2- oxidation at the reaction plane.展开更多
The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0....The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.展开更多
Au-Pt/SnO2/GC composite electrode was prepared by self-assembling Au-Pt nanoparticles on SnO2 film, which was deposited on actived glassy carbon （GC）. Atomic force microscopy （AFM） and scanning electron microscopy...Au-Pt/SnO2/GC composite electrode was prepared by self-assembling Au-Pt nanoparticles on SnO2 film, which was deposited on actived glassy carbon （GC）. Atomic force microscopy （AFM） and scanning electron microscopy （SEM） images revealed that dense and uniform Au-Pt particles with 25-nm diameter were dispersed on SnO2 film. X-ray photoelectron spectroscopy （XPS） results proved that there was an interaction between Au-Pt nanoparticles and SnO2 support. Electrochemical experiments showed that Au-Pt/SnOz/GC composite electrode had a good electrocatalytic activity to the oxidation of methanol展开更多
The electrochemical quartz crystal microbalance (EQCM) was applied to study the electrochemical behaviors of polycrystalline Au in sulfuric acid solution. The large mass change observed in the doublelayer region was a...The electrochemical quartz crystal microbalance (EQCM) was applied to study the electrochemical behaviors of polycrystalline Au in sulfuric acid solution. The large mass change observed in the doublelayer region was attributed to the partly discharged adsorption of sulfate anions with the co-adsorption of H2O. According to the observed EQCM frequency response, the formation mechanism of surface oxide was reasonably postulated, in which the roles of the adsorbed anions and the co-adsorbed H2O were particularly emphasized.展开更多
The electrochemical quartz crystal impedance system (EQCIS) has been used for the study of a partially immersed Au electrode in 0.2 mol/L NaClO4 aqueous solution. The influences of the immersed area and height of the ...The electrochemical quartz crystal impedance system (EQCIS) has been used for the study of a partially immersed Au electrode in 0.2 mol/L NaClO4 aqueous solution. The influences of the immersed area and height of the electrode on the EQCIS responses were evaluated, showing the highest response sensitivity to liquid loading at the center of the piezoelectric quartz crystal electrode. The increase in the immersed height of the Au electrode at oxygen reduction potentials during potential cycling was measured by this technique.展开更多
110 nm-thick Au layers were sputter-deposited on unheated glasses coatedabout a 10 nm-thick and a 50 nm-thick Cr layer respectively. The Au/Cr bilayer films were annealedin a vacuum of 1 mPa at 300℃ for 2, 5 and 30 m...110 nm-thick Au layers were sputter-deposited on unheated glasses coatedabout a 10 nm-thick and a 50 nm-thick Cr layer respectively. The Au/Cr bilayer films were annealedin a vacuum of 1 mPa at 300℃ for 2, 5 and 30 min, respectively. Auger electron spectroscopy, X-raydiffraction and Field emission scanning electron microscopy were used to analyze the composition andstructure of the Au layers. The resistivity of the bilayer films was measured by using four-pointprobe technique. The adhesion of the bilayer films to the substrate was tested using tape tests. Theamount of Cr atoms diffusing into the Au layer increases with increasing the annealing time,resulting in a decrease in lattice constant and an increase in resistivity of the Au layer. Thecontent of Cr inside the Au layer grown on the thinner Cr layer is less than that grown on thethicker Cr layer. For the Au/Cr bilayer films, the lower resistivity and the good adhesion to theglass substrate can be obtained at a shorter annealing time for a thinner Cr layer.展开更多
基金V, ACKNOWLEDGMENTS This work was supported by one Hundred Talents＇ Program of the Chinese Academy of Science, the National Natural Science Foundation of China （No.21073176）, and 973 Program from the Ministry of Science and Technology of China （No.2010CB923302）.
文摘The temperature dependence of hydrogen evolution reaction （HER） at a quasi-single crystalline gold electrode in both 0.1 mol/L HCl04 and 0.1 mol/L KOH solutions was investigated by cyclic voltammetry. HER current displays a clear increase with reaction overpotential （η） and temperature from 278-333 K. In 0.1 mol/L HClO4 the Tafel slopes are found to increases slightly with temperature from 118 mV/dec to 146 mV/dec, while in 0.1 mol/L KOH it is ca. 153±15 mV/dec without clear temperature-dependent trend. The apparent activation energy （Ea） for HER at equilibrium potential is ca. 48 and 34 kJ/mol in 0.1 mol/L HC104 and 0.1 mol/L KOH, respectively. In acid solution, Ea decreases with increase in η, from Ea-37 kJ/mol （η=0.2 V） to 30 kJ/mol （η=0.35 V）. In contrast, in 0.1 mol/L KOH, Ea does not show obvious change with U. The pre-exponential factor （A） in 0.1 mol/L HC104 is ca. 1 order higher than that in 0.1 mol/L KOH. Toward more negative potential, in 0.1 mol/L HC104 A changes little with potential, while in 0.1 mol/L KOH it displays a monotonic increase with U. The change trends of the potential-dependent kinetic parameters for HER at Au electrode in 0.1 mol/L HClO4 and that in 0.1 mol/L KOH are discussed.
基金supported by the National Natural Science Foundation of China(No.21473175 and No.21273215)the National Key Basic Research Program of China from the Ministry of Science andTechnology of China(No.2015CB932301)
文摘The hydrogen peroxide oxidation reaction (HPOOR) on Au(111) electrode in alkaline solutions with pH values ranging from 10 to 13 was examined systematically. HPOOR activity increased and the slope of the i-E curve decreased with increasing pH. HO2- is suggested to be the main reactive intermediate for HPOOR in alkaline media. The fast kinetics for HPOOR in alkaline solution is facilitated by the electrostatic interaction between the positively charged electrode and the reactive anions (i.e., HO2- and HO-), which increases the concentration of these reactants and the thermodynamic driving force for HO2- oxidation at the reaction plane.
基金Supported by the National Natural Science Foundation of China(No.20605009)
文摘The direct electron transfer of hemoglobin at the PAMAM-MWNTs-AuNPs composite film modified glassy carbon electrode was studied. In a phosphate buffer solution（PBS, pH=7.0）, the formal potential（E^0） of Hb was -0.105 V versus SCE, the electron transfer rate constant was 4.66 s-1. E^0＇ of Hb at the modified electrode was linearly varied in a pH range of 5.0-8.0 with a slope of-49.2 mV/pH. The Hb/PAMAM-MWNTs-AuNPs/GCE gave an excellent electrocatalytic response to the reduction of hydrogen peroxide. The catalytic current increased linearly with H2O2 concentration in a range of 1.0× 10^-6 to 2.2× 10^-3 mol/L. The detection limit was 2.0× 10^-7 mol/L at a signal to noise ratio of 3. The Michaelis-Menten constant（Km^app） was 2.95 mmol/L.
基金supported by the High-Tech Research and Development Program of China (No. 2007AA03Z219)the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality, and the Beijing Natural Science Foundation (No. 207001)
文摘Au-Pt/SnO2/GC composite electrode was prepared by self-assembling Au-Pt nanoparticles on SnO2 film, which was deposited on actived glassy carbon （GC）. Atomic force microscopy （AFM） and scanning electron microscopy （SEM） images revealed that dense and uniform Au-Pt particles with 25-nm diameter were dispersed on SnO2 film. X-ray photoelectron spectroscopy （XPS） results proved that there was an interaction between Au-Pt nanoparticles and SnO2 support. Electrochemical experiments showed that Au-Pt/SnOz/GC composite electrode had a good electrocatalytic activity to the oxidation of methanol
文摘The electrochemical quartz crystal microbalance (EQCM) was applied to study the electrochemical behaviors of polycrystalline Au in sulfuric acid solution. The large mass change observed in the doublelayer region was attributed to the partly discharged adsorption of sulfate anions with the co-adsorption of H2O. According to the observed EQCM frequency response, the formation mechanism of surface oxide was reasonably postulated, in which the roles of the adsorbed anions and the co-adsorbed H2O were particularly emphasized.
基金This work was supported by the National Natural Science Foundation of China the Science and Technology Foundation of Hunan P
文摘The electrochemical quartz crystal impedance system (EQCIS) has been used for the study of a partially immersed Au electrode in 0.2 mol/L NaClO4 aqueous solution. The influences of the immersed area and height of the electrode on the EQCIS responses were evaluated, showing the highest response sensitivity to liquid loading at the center of the piezoelectric quartz crystal electrode. The increase in the immersed height of the Au electrode at oxygen reduction potentials during potential cycling was measured by this technique.
文摘110 nm-thick Au layers were sputter-deposited on unheated glasses coatedabout a 10 nm-thick and a 50 nm-thick Cr layer respectively. The Au/Cr bilayer films were annealedin a vacuum of 1 mPa at 300℃ for 2, 5 and 30 min, respectively. Auger electron spectroscopy, X-raydiffraction and Field emission scanning electron microscopy were used to analyze the composition andstructure of the Au layers. The resistivity of the bilayer films was measured by using four-pointprobe technique. The adhesion of the bilayer films to the substrate was tested using tape tests. Theamount of Cr atoms diffusing into the Au layer increases with increasing the annealing time,resulting in a decrease in lattice constant and an increase in resistivity of the Au layer. Thecontent of Cr inside the Au layer grown on the thinner Cr layer is less than that grown on thethicker Cr layer. For the Au/Cr bilayer films, the lower resistivity and the good adhesion to theglass substrate can be obtained at a shorter annealing time for a thinner Cr layer.
