In this article, the electrochemical performance of the electrodes of zinc polycrystal, Zn(002) and Zn(100) single crystals were studied by the Tafel line extrapolation of the potentio-dynamic polarization curves,...In this article, the electrochemical performance of the electrodes of zinc polycrystal, Zn(002) and Zn(100) single crystals were studied by the Tafel line extrapolation of the potentio-dynamic polarization curves, the cyclic voltammetry and the charge/discharge experiment. The results shows that in 6.0 mol·L^-1 KOH solution the corrosion rate of Zn polycrystal, Zn(100) and Zn(002) single crystals decreases in turn; and the reversibility and the charge/discharge performance of Zn single crystal was superior to Zn polycrystal. The dendrite growth of the surface of Zn polycrvstal was easier than Zn single crystal during the stages of charge/discharge.展开更多
Variable temperature in situ FTIR spectroscopy has been used as the primary tool to investigate the effects of temperature(10 to 50 ℃) on formaldehyde dissociative adsorption and electro oxidation on the Ru(00...Variable temperature in situ FTIR spectroscopy has been used as the primary tool to investigate the effects of temperature(10 to 50 ℃) on formaldehyde dissociative adsorption and electro oxidation on the Ru(0001) electrode in perchloric acid solution, and the results were interpreted in terms of the surface chemistry of the Ru(0001) electrode and compared to those obtained during our previous studies on the adsorption of CO under the same conditions. It was found that formaldehyde did undergo dissociative adsorption, even at -200 mV vs . Ag/AgCl, to form linear(CO L) and 3 fold hollow(CO H) binding CO adsorbates. In contrast to the adsorption of CO, it was found that increasing the temperature to 50 ℃ markedly increased the amount of CO adsorbates formed on the Ru(0001) surface from the adsorption of formaldehyde. On increasing the potential, the electro oxidation of the CO adsorbates to CO 2 took place via reaction with the active (1×1) O oxide. A significant increase in the surface reactivity was observed on the RuO 2(100) phase formed at higher potentials. Formic acid was detected as a partial oxidation product during formaldehyde electro oxidation. The data obtained at 50 ℃ are markedly different from those collected at 10 and 25 ℃ in terms of the amount of both CO 2 and formic acid formed and the adsorbed CO L and CO H species observed. These results were rationalized by the thermal effects on both the loosening of the CO adlayer and the activation of surface oxide on increasing the temperature.展开更多
Surface processes of CO_(2)reduction on Pt(210),Pt(310),and Pt(510)electrodes were studied by cyclic voltammetry.Different surface structures of these platinum single crystal electrodes were obtained by various treatm...Surface processes of CO_(2)reduction on Pt(210),Pt(310),and Pt(510)electrodes were studied by cyclic voltammetry.Different surface structures of these platinum single crystal electrodes were obtained by various treatment conditions.The experimental results illustrated that the electrocatalytic activity of Pt single crystal electrodes towards CO_(2)reduction is decreased in an order of Pt(210)>Pt(310)>Pt(510),i.e.,with the decrease of(110)step density on well-defined surfaces.When the surfaces were reconstructed due to oxygen adsorption,the catalytic activity of all the three electrodes has been enhanced to a cer-tain extent.Although the activity order remains unchanged,the electrocatalytic activity has been en-hanced more significantly as the density of(110)step sites is more intensive on the Pt single crystal surface.It has revealed that the more open the surface structure is,the more active the Pt single crystal electrode will be,and the easier for the electrode to be transformed into a surface structure that exhib-its higher activity under external inductions.However,the relatively ordered surfaces of Pt single crystal electrode are comparatively stable under the same external inductions.The present study has gained knowledge on the interaction between CO_(2)and Pt single crystal electrode surfaces at a micro-scopic level,and thrown new insight into understanding the surface processes of electrocatalytic re-duction of CO_(2).展开更多
文摘In this article, the electrochemical performance of the electrodes of zinc polycrystal, Zn(002) and Zn(100) single crystals were studied by the Tafel line extrapolation of the potentio-dynamic polarization curves, the cyclic voltammetry and the charge/discharge experiment. The results shows that in 6.0 mol·L^-1 KOH solution the corrosion rate of Zn polycrystal, Zn(100) and Zn(002) single crystals decreases in turn; and the reversibility and the charge/discharge performance of Zn single crystal was superior to Zn polycrystal. The dendrite growth of the surface of Zn polycrvstal was easier than Zn single crystal during the stages of charge/discharge.
文摘Variable temperature in situ FTIR spectroscopy has been used as the primary tool to investigate the effects of temperature(10 to 50 ℃) on formaldehyde dissociative adsorption and electro oxidation on the Ru(0001) electrode in perchloric acid solution, and the results were interpreted in terms of the surface chemistry of the Ru(0001) electrode and compared to those obtained during our previous studies on the adsorption of CO under the same conditions. It was found that formaldehyde did undergo dissociative adsorption, even at -200 mV vs . Ag/AgCl, to form linear(CO L) and 3 fold hollow(CO H) binding CO adsorbates. In contrast to the adsorption of CO, it was found that increasing the temperature to 50 ℃ markedly increased the amount of CO adsorbates formed on the Ru(0001) surface from the adsorption of formaldehyde. On increasing the potential, the electro oxidation of the CO adsorbates to CO 2 took place via reaction with the active (1×1) O oxide. A significant increase in the surface reactivity was observed on the RuO 2(100) phase formed at higher potentials. Formic acid was detected as a partial oxidation product during formaldehyde electro oxidation. The data obtained at 50 ℃ are markedly different from those collected at 10 and 25 ℃ in terms of the amount of both CO 2 and formic acid formed and the adsorbed CO L and CO H species observed. These results were rationalized by the thermal effects on both the loosening of the CO adlayer and the activation of surface oxide on increasing the temperature.
基金Supported by the National Natural Science Foundation of China(Grant Nos.20673091,20433060 and 20373059)the Special Funds for Major State Basic Research Project of China(Grant No.2002CB211804)
文摘Surface processes of CO_(2)reduction on Pt(210),Pt(310),and Pt(510)electrodes were studied by cyclic voltammetry.Different surface structures of these platinum single crystal electrodes were obtained by various treatment conditions.The experimental results illustrated that the electrocatalytic activity of Pt single crystal electrodes towards CO_(2)reduction is decreased in an order of Pt(210)>Pt(310)>Pt(510),i.e.,with the decrease of(110)step density on well-defined surfaces.When the surfaces were reconstructed due to oxygen adsorption,the catalytic activity of all the three electrodes has been enhanced to a cer-tain extent.Although the activity order remains unchanged,the electrocatalytic activity has been en-hanced more significantly as the density of(110)step sites is more intensive on the Pt single crystal surface.It has revealed that the more open the surface structure is,the more active the Pt single crystal electrode will be,and the easier for the electrode to be transformed into a surface structure that exhib-its higher activity under external inductions.However,the relatively ordered surfaces of Pt single crystal electrode are comparatively stable under the same external inductions.The present study has gained knowledge on the interaction between CO_(2)and Pt single crystal electrode surfaces at a micro-scopic level,and thrown new insight into understanding the surface processes of electrocatalytic re-duction of CO_(2).