摘要
现场红外反射光谱电化学是红外光谱与电化学方法相结合而形成的一种学科交叉研究方法。其特点是同时获得电化学和红外光谱信息,为现场监测反应中间体、吸附物种及反应产物提供了非常有利的研究手段,因而在电化学反应、表面吸脱附过程等研究中得到广泛的应用。提供了大量关于固/液界面分子水平的信息,在推动电化学科学研究进入分子水平中发挥了重要作用。
衰减全反射红外光谱技术是表层结构分析的有利手段。与传统透射制样法相比,具有非破坏性,适用于溶液样品测量,简单方便等优点。衰减全反射红外光谱可有效地排除溶剂吸收的影响,提供表面化学信息。适用于界面现象研究及现场监测溶液中化学或生物反应过程。本文在文献基础上,运用现场红外反射光谱电化学和衰减全反射红外光谱法对电化学反应机理及界面吸脱附过程进行了研究。主要内容如下:
1.综述了现场红外反射光谱电化学和衰减全反射红外光谱技术的原理、方法及应用进展。
2.运用循环伏安法和现场红外反射光谱电化学技术,研究了0.2mol L~(-1) KCI水溶液中对-甲氨基苯酚在铂电极上的电氧化还原过程。循环伏安扫描和现场红外反射吸收光谱结果表明:对-甲氨基苯酚的电氧化还原过程中有两个电子和两个质子发生转移,对-甲氨基苯酚首先氧化生成对-甲亚胺基苯醌,然后其氧化产物发生不可逆水解反应生成对苯醌和甲氨。
3.现场红外反射光谱电化学和循环伏安法研究吡哆醇在碱性溶液中金电极上的电氧化过程。电化学循环伏安结果表明在0.1mol L~(-1) NaOH溶液中,Au电极对吡哆醇有很高的催化活性,吡哆醇的氧化是不可逆的,近似于一级
In situ infrared reflection spectroelectrochemisty, which is the combination of infrared spectroscopy and electrochemistry, can provide infrared spectral and electrochemical information at the same time. It has become a powerful tool for in situ determining the intermediate, adsorbed species and products of electrode reaction. And it has been widely used to study electrocatalytic oxidation mechanism and adsorption/desorption process. This information gives valuable data for a molecular picture of solid/liquid interface and contributes to the study of electrochemical process at a molecular level.Attenuated total reflection infrared spectroscopy (ATR) is a useful tool for surface analysis providing structural and chemical information about the sample. Compared with the traditional transmission IR techniques, the method has several advantages including non-destruction, aqueous sample analysis, and convenience. ATR spectroscopy can yield valuable surface-chemical data with reduced interferences from solvent, which allows exploring solid/liquid interfacial phenomena and monitoring chemical or biological reaction in situ. The studies in this thesis are summarized as follows:1. The principle, method and the recent progress of in situ infrared reflection spectroelectrochemisty and attenuated total reflection infrared spectroscopy technique is reviewed.2. The electrochemical redox reaction of p-methylaminophenol on platinum electrode in 0.2 mol L~(-1) KC1 solution was investigated by cyclic voltammetry and in situ reflection absorption Fourier transform infrared spectroscopy (FTIRS).
The results show that two electrons and protons were transferred during the redox process of p-methylaminophenol. The electrochemical oxidation of p-methylaminophenol yields /?-N-methylobenzoquinoeimin intermediate at first. And the resulted p-N-methylobenzoquinoeimin further undergoes irreversible hydrolysis to yield /?-benzoquinone and methylamine.3. The electrochemical oxidation of pyridoxol (PN) on a poly crystal line gold electrode was investigated by cyclic voltammetry and in situ Fourier transform infrared spectroscopy (FTIRS). In 0.1 M aqueous NaOH, the gold electrode showed a high catalytic activity for the irreversible oxidation of PN via an approximate first-order kinetic process. The individual ionic species and the major tautomeric equilibria of PN molecules in aqueous solutions were evidenced well from the pH-dependent attenuated total internal reflection (ATR) spectra, and the results were in good agreement with the voltammetric observations. In situ single potential alteration reflectance spectroscopy (SPAIRS) demonstrated that a lactone form of PN, rather than pyridoxal aldehyde, was likely formed, which was subsequently diffused into thin layer solution and underwent hydrolysis slowly to pyridoxic acid (PA) as the final product. In addition, the adsorption of PN at Au electrode was characterized by in situ subtractively normalized interfacial Fourier transform spectroscopy (SNIFTIR) method, which revealed that the adsorption of deprotonated PN, via nitrogen atom in vertical configuration on electrode surface, occurred from -0.5 V vs Ag|AgCl|KCl(sat), which was much lower than the potential of PN electrooxidation observed from ca. 0 V.
引文
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