EQCM and in-situ reflectance FTIR spectroscopic studies of adsorption and oxidation of methanol on Pt electrode in alkaline media

The adsorption and oxidation of methanol on Pt electrode in alkaline media have been investigated by using cyclic voltammetry, electrochemical quartz crystal microbalance (EQCM) and in-situ reflectance FTIR spectroscopy. The experimental results demonstrated that the electrooxidation of CH3OH was closely relative to solution acidity. Only one current peak of methanol oxidation in PGPS was detected at -0.09 V, which illustrated the disappearance of the second current peak due to Pt electrode passivation in alkaline media. The magnitude of the dissociative adsorbate of methanol in alkaline media is smaller than that in acidic media. The main product, such as CO2 and CO32-, was detected clearly and the reactive intermediates that were determined by FTIRS under experimental condition might be mainly HCOO- species. The EQCM studies provide quantitative results of surface mass changes during methanol oxidation, and have thrown new light in the elucidating methanol oxidation

Study on Electrocatalytic Oxidation of sec-Butyl Alcohol on Pt Electrode Modified with Adatoms

运用电化学循环伏安和石英晶体微天平研究了HClO4溶液中仲丁醇在Pt电极及以Sb和S吸附原子修饰的Pt(Pt/Sbad和Pt/Sad)电极上的电催化氧化过程 .从电极表面质量变化可以看出 ,仲丁醇的氧化与电极表面的氧物种有着极其密切的关系 .Pt电极表面Sb吸附原子可在较低的电位下吸附氧 ,明显提高仲丁醇的氧化活性 .与Pt电极相比 ,Sb吸附原子修饰的Pt电极使仲丁醇氧化的峰电位负移约 10 0mV .相反 ,Pt电极表面S吸附原子的氧化会消耗表面氧物种 ,抑制仲丁醇的氧化 .从电极表面质量变化提供了吸附原子电催化作用的数据The processes of adsorption and oxidation of sec butyl alcohol on Pt electrode and Pt electrodes modified with Sb and S (Pt/Sb ad and Pt/S ad ) were studied by using cyclic voltammetry and electrochemical quartz crystal microbalance (EQCM). The results demonstrated that the oxidation of sec butyl alcohol depends strongly on oxidation states of electrode surface. Sb adatoms on Pt surface can adsorb oxygen at relatively low potentials, and exhibit catalytic effects for sec butyl alcohol oxidation. In comparison with the case of Pt electrode, the oxidation peak potential of sec butyl alcohol on Pt surface modified with Sb was negatively shifted about 100 mV. On the contrary, the oxidation of S adatoms consumes oxygen species on Pt electrode surface. As a consequence, the oxidation of sec butyl alcohol was inhibited by the presence of S ad . The EQCM studies provided quantitative results of surface mass changes during sec butyl alcohol oxidation, and have thrown new light on elucidating different effects of adatoms Sb ad and S ad on Pt electrode towards sec butyl alcohol oxidation.国家自然科学基金 (2 983 3 0 60 );; 教育部博士点专项科研基金 (19990 3 840 3 );; 福建省教委科研基金资助项目 (K2 0 0 110 1

Adsorption and Oxidation of 1,3-Butanediol on Pt and Sb,S Modified Pt Electrodes

应用电化学循环伏安和石英晶体微天平 (EQCM )研究了 1 ,3 -丁二醇 ( 1 ,3 -BDL )在Pt电极和以Sb、S吸附原子修饰的Pt(Pt/Sbad和Pt/Sad)电极上的吸附和氧化过程。从电极表面质量变化的结果分析 ,可认为 1 ,3 -丁二醇的氧化与电极表面氧物种有着极其密切的关系。Pt电极表面Sb吸附原子能在较低的电位下吸附氧 ,可显著提高 1 ,3 -丁二醇电催化氧化活性。与Pt电极相比较 ,饱和吸附Sb原子的Pt电极 ,1 ,3 -丁二醇氧化的峰电位负移了 0 2 5V ,峰电流增加了近 1倍。相反 ,Pt电极表面S吸附原子的氧化会消耗表面氧物种 ,饱和吸附S原子的Pt电极上 1 ,3 -丁二醇的电氧化受到抑制。本文从表面质量变化提供了吸附原子电催化作用的新数据。The processes of adsorption and oxidation of 1,3-butanediol on Pt and Pt modified with Sb and S in saturation(Pt/Sb ad and Pt/S ad )electrodes were studied by using cyclic voltammetry and electrochemical quartz crystal microbalance(EQCM).The results demonstrated that the oxidation of 1,3-butanediol depended strongly on oxidation states of electrode surface.Sb adatoms on Pt surface could adsorb oxygen at relatively low potentials,and exhibited catalytic effects for 1,3-butanediol oxidation.In comparison with the case of Pt electrode,the oxidation peak potential of 1,3-butanediol on Pt surface modified with Sb in saturation was negatively shifted about 250 mV with peak current being doubly increased.In a contrary,the oxidation of S adatoms consumed oxygen species of Pt electrode surface.As a consequence,the oxidation of 1,3-butanediol was inhibited on Pt surface modified with S in saturation.The EQCM studies provided quantitative results of surface mass changes during 1,3-butanediol oxidation,and threw new light in elucidating different effects of adatoms Sb ad and S ad on Pt electrode surface towards 1,3-butanediol oxidation.国家自然科学基金 (2 983 3 0 60 );; 福建省教委科研基金资助项目 (K2 0 0 110 1

碱性介质中甲醇在铂电极表面吸附和氧化的电化学原位FTIR反射光谱和EQCM研究

运用电化学循环伏安、原位FTIR反射光谱和石英晶体微天平(EQCM)等方法研究了碱性介质中甲醇在Pt电极表面吸附和氧化行为.结果表明:甲醇电氧化与溶液酸碱性有密切的关系.酸性介质中甲醇在Pt电极上的CV曲线有两个正向氧化峰,而碱性介质中只有一个正向氧化峰,第二个氧化峰的消失可能是由于碱性介质中Pt电极在高电位下形成高氧化态的氧物种毒化其表面引起的.碱性介质中甲醇解离吸附产物的数量比酸性介质的明显减少,对甲醇氧化的第一个氧化峰表现出更高的电催化活性.目前实验条件下,原位FTIR反射光谱检测到:碱性介质中甲醇电氧化的最终产物是CO_2和CO_3~(2-),反应中间体主要为HCOO~-物种.从电极表面质量定量变化的角度提供了甲醇反应机理的新数据

碱性介质中正丁醇在铂电极上吸附和氧化的电化学原位FTIR反射光谱和EQCM研究

运用电化学循环伏安(CV)、原位FTIR反射光谱和电化学石英晶体微天平(EQCM)等方法研究了碱性介质中正丁醇在Pt电极表面吸附和氧化行为。结果表明:正丁醇电氧化过程与溶液酸碱性有着密切的关系。酸性介质中正丁醇在Pt电极上的CV曲线有2个正向氧化峰,而碱性介质中只有1个正向氧化峰,第2个氧化峰的消失可能是由于碱性介质中Pt电极表面钝化引起的。原位FTIR反射光谱检测到,在实验条件下,碱性介质中正丁醇电氧化过程的最终产物只有丁酸根。EQCM研究还从电极表面质量定量变化的角度提供了正丁醇反应机理的新数据

Study on electrocatalytic oxidation of sec-butyl alcohol on pt electrode modified with adatoms

The processes of adsorption and oxidation of sec-butyl alcohol on Pt electrode and Pt electrodes modified with Sb and S (Pt/Sb-ad and Pt/S-ad) were studied by using cyclic voltammetry and electrochemical quartz crystal microbalance (EQCM). The results demonstrated that the oxidation of sec-butyl alcohol depends strongly on oxidation states of electrode surface. Sb adatoms on Pt surface can adsorb oxygen at relatively low potentials, and exhibit catalytic effects for sec-butyl alcohol oxidation, In comparison with the case of Pt electrode, the oxidation peak potential of sec-butyl alcohol on Pt surface modified with Sb was negatively shifted about 100 mV. On the contrary, the oxidation of S adatoms consumes oxygen species on Pt electrode surface. As a consequence, the oxidation of sec-butyl alcohol was inhibited by the presence of S-ad. The EQCM studies provided quantitative results of surface mass changes during sec-butyl alcohol oxidation, and have thrown new light on elucidating different effects of adatoms Sb-ad and S-ad on Pt electrode towards sec-butyl alcohol oxidation

The adsorption and oxidation of isopropanol at platinum electrode in alkaline media

The adsorption and oxidation of isopropanol in alkaline media at platinum electrode have been investigated by using electrochemical quartz crystal microbalance (EQCM) and in situ FTIR spectroscopy. The results show that there is no self-poisoning in the electrooxidation of isopropanol in alkaline media. Though no poison species, such as CO, are evidenced by in situ FTIR spectroscopy, the adsorption of isopropanol or its dissociative products on Pt surface is suggested by EQCM data. The final product of isopropanol oxidation is only acetone under experimental condition, which suggests that the oxidation of isopropanol into acetone takes place via dehydrogenation step. The EQCM studies provide quantitative results of surface mass variation and have thrown new light in the elucidating isopropanol oxidation

Man-ka, Da-dao-cheng, Tamsui Port: The three kinds of settlement pattern and cultural factors of port-town in Taiwan during the Qing Dynasty

清中叶以后，北台湾的淡水河流域汉人移民人口逐渐增加，将闽南地区的宗教信仰和建筑风格带入此地，使得地方聚落开始快速发展。在清末以后，开港通商成为了东亚最大的茶叶和樟脑出口地，西方殖民者、传教士将基督教和西方文化引进此地。由于淡水河是当时北台湾最主要的联外交通，从这些地区的建筑型态和宗教信仰来看，可明显地看出是外来文化影响最深并且多元文化融合程度最高之地区。 艋舺地区是清领前期汉人商业聚落的代表性地区，清末以前是北台湾对大陆主要贸易港市，根据当地移民带来的神灵信仰和街屋建筑，可明显的看出其受闽南地区的重要影响。清末以后，艋舺因种种因素而走向没落，但是对外的交流仍然持续着，不只面向闽南地区的文化交...After the middle period of Qing Dynasty, the Han immigrant population of the Tamsui River Basin in northern Taiwan was gradually increased, they brought the Minnan religious belief and architectural style into the place, and the settlements developed rapidly. When Tamsui Port opened in late Qing Dynasty, this area became the largest tea and camphor exports port in East Asia, the Western colonizers...学位：历史学硕士院系专业：人文学院历史学系_考古学及博物馆学学号：1032009115416