Ag(I)与Co(II)离子对阳极析氧过程的电催化作用

Influence of Ag(Ⅰ), Co(Ⅱ) and Ni(Ⅱ) ions on oxygen anodic evolution at Pt and Ti/Pt/PbO2 electrodes was investigated in surphuric acid solutions. The oxygen evolution reaction at Ti/Pt/PbO2 electrode in surphuric acid solutions is characterized by two linearφ~ lgi relationships. At low c.d. it is close to 2.303RT/(1+β)F, whereas at high c.d. it is close to 2.303RT/βF. In the presence of Ag(Ⅰ) or Ni(Ⅱ) ions in the electrolytic solution the Tafel slope of oxygen evolution tends to be low, 2.303RT/(1+β)F (withβ=0.5). However, the oxygen evolution reaction at Pt electrodes in H2SO4 or CoSO4﹢H2SO4 solutions is characterized by one linearφ~ lgi relationship. The Tafel slope is close to 2.303RT/βF. In the presence of Ag(Ⅰ) or Ni(Ⅱ) ions in the electrolytic solution the Tafel slope of oxygen evolution tends to be low, 2.303RT/(1+β)F. The oxygen anodic evolution reactions are catalyzed by Ag(Ⅰ), Co(Ⅱ) and Ni(Ⅱ) ions in the electrolytic solution. When Ag(Ⅰ) or Ni(Ⅱ) was mixed with Co(Ⅱ), a promising catalyst for oxygen anodic evolution with higher catalyst activity than either of them alone was found. A comparison of the PbO2 electrode and the Pt electrode has also been given.     

硫酸溶液中Ce^3＋离子在PbO2电极上阳极氧化过程动力学

用“分解极化曲线”法研究ＰｂＯ２电极上Ｃｅ＾４＋阳极形成的动力学。测得电位在１．７￣１．９Ｖ（ｖｓ．ＳＣＥ）区域和高于１．９Ｖ区域的Ｏ２和Ｃｅ＾４＋的极化曲线的Ｔａｆｅｌ斜率和两者的动力学方程。推测了ＰｂＯ２电极上Ｃｅ＾４＋形成和Ｏ２析出的机理及两区域内反应机理的差别。所推得的动力学方程均与实验相符。     

β-PbO2纳米棒及Pb3O4纳米晶的制备与表征

利用NaClO在碱性溶液中与Pb(Ac)2进行氧化反应直接合成出直径为10－20nm、长度为400nm、长径比达20以上的纯相β－PbO2纳米棒，对所得β－PbO2在420℃下进行热解，得到晶粒尺寸为20nm左右的Pb3O4。对液相氧化反应的温度、时间、氧化剂浓度、pH等因素的影响进行了详细研究，获得了最佳合成反应条件，所得产物利用粉末X射线衍射和透射电子显微镜分析进行了表征。     

Degradation of Phenol by Hydroxyl Radicals on Different Coating Lead Dioxide Electrodes

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.     

太阳能选择性吸收涂层PbO2的性能研究

本文主要研究制备方法对改变二氧化铅(PbO2)纳米涂层的太阳光谱吸收选择性的影响.通过恒电流沉积法制备PbO2纳米涂层,并通过改变制备条件以得出最佳光谱吸收选择性,并对该吸收涂层进行了紫外-可见光谱(Uv-vis),傅里叶红外光谱(FTIR),扫描电子显微镜(SEM),透射电子显微镜(TEM)等对涂层性能和结构进行分析...     

氧化铅掺杂碳纳米管糊预氧化电流型葡萄糖生物传感器的研究

以掺杂预氧化物质(二氧化铅)、电子介体(二茂铁羧酸)和碳纳米管作电极材料,研制预氧化电流型葡萄糖生物传感器.碳纳米管糊中掺入二氧化铅可消除抗坏血酸、尿酸等还原性物质对葡萄糖测定的干扰,该传感器在+0.40 V(vs.SCE)的工作电位下仍保持良好的抗干扰能力(对含有1.0 mmo.lL-1的葡萄糖溶液,1.8 mmo.lL-1的抗坏血酸和2.2 mmo.lL-1的尿酸均不产生干扰)和较快的响应速率(10 s),响应电流与葡萄糖浓度在0.50~20 mmo.lL-1范围内呈良好的线性关系,相关系数为0.9987.此传感器用于人体血清中葡萄糖的测定,结果满意.     

SnO_2 Sb_2O_3中间层的制备条件对Ti/SnO_2 Sb_2O_3/PbO_2阳极性能的影响

研究了聚合前驱体制备的SnO2 Sb2 O3 中间层的焙烧温度、锑含量对Ti/SnO2 Sb2 O3 /PbO2 阳极性能的影响。用XRD、ESEM和探针法对锡锑中间层进行了表征 ,应用阳极寿命快速检测法测定了Ti/SnO2 Sb2 O3 /PbO2 电极在 1 0mol/LH2 SO4溶液中的寿命 ,并用极化曲线和电荷容量表征了锡锑中间层对钛基PbO2 阳极性能的影响。实验结果表明 ,聚合前驱体制备中间层的焙烧温度和锑含量对Ti/SnO2 Sb2 O3 /PbO2 电极的寿命和性能有显著的影响。在锡锑中间层的制备温度为 5 0 0℃、n(Sn)∶n(Sb) =9∶1时 ,制得的Ti/SnO2 Sb2 O3 /PbO2 电极用阳极寿命快速检测法测得的电极寿命达 30h ,具有良好的稳定性     

添加剂对电沉积二氧化铅阳极性能的影响

本文研究了各种添加剂对电沉积二氧化铅阳极性能的影响,结果表明卤素离子和过渡金属离子对制备二氧化铅阳极的形貌和性能有很大影响,实验发现以氯离子和铁离子为添加剂制备的二氧化铅阳极用于电解析出臭氧时,其活性和稳定性明显改善。     

改性金属氧化物电极用于降解邻甲酚的性能研究

采用电沉积法制备了Ti/Ti O2-NTs/Pb O2、Ti/Ti O2-NTs/Ce-Pb O2、Ti/Ti O2-NTs/Fe-Pb O2三种电极,采用X射线衍射(XRD)、线性伏安扫描(LSV)、电极加速寿命等手段分别对所制备电极进行了表征,并以邻甲酚作为目标污染物评价了电极的电催化活性。研究结果表明,被Fe、Ce修饰后的两种Pb O2电极的析氧电位、稳定性、电催化活性均高于未修饰电极,且所制备的三种电极的活性催化层均为β型Pb O2,邻甲酚在三种电极上的电催化降解反应均遵守一级反应动力学规律。其中被Fe修饰的Pb O2电极是降解邻甲酚综合性能最佳的电极,该电极析氧电位为2.12 V,当电流密度为10 m A/cm2时对邻甲酚去除率为99.74%,COD去除率为60.31%,加速寿命是未修饰电极的2.6倍。     

钛基二氧化铅电极上氯析出过程的研究

用极化曲线法研究了钛基二氧化铅电极(β-PbO_2)在NaCl溶液中的阳极析氯过程。结果表明,反应速度与Cl~-离子浓度成正比,H~ 离子通过OH~-离子的竞争吸附对析氯过程起促进作用。电极转速对阳极极化曲线没有影响,说明扩散过程不起控制作用。稳态动力学数据指出,氯的析出机理符合电化学放电规律,速度控制步骤为:MCl~-_(adi)→MCl~-_(adi e)。