原位同步辐射红外关联谱学技术研究界面电化学反应过程

Application of synchrotron radiation in biologicIn situ synchrotron radiation infrared correlated spectroscopy study on the dynamic process of interfacial electrochemical reactionsal imaging analysis

电化学界面动力学决定了所有电化学反应性质.从原子和分子水平上多维度原位观察电极的表界面电化学反应动态过程对于典型的电化学储能技术(电解槽、燃料电池)中催化剂的结构设计、合成和筛选具有重要意义,但是复杂的电化学界面以及微量、快速的反应中间态信号给界面电化学反应动态过程研究带来了极大的挑战.同步辐射傅里叶变换红外光谱(SR-FTIR)具有独特的分子指纹识别功能,可以用来确定电化学界面的活性物质,结合对纳米材料的局部原子结构高度敏感的同步辐射X射线吸收精细结构(SR-XAFS)光谱可以开展界面电化学反应过程的实时动态研究,有助于指导设计用于高效高能量密度能源系统的先进电催化剂.本文基于近年来本课题组的研究工作,系统地介绍了获得高质量的电化学反应过程中同步辐射红外关联谱学实验结果的策略,及其应用于电催化反应动态过程研究成果,其中主要选用当前热门的金属有机框架(MOF)纳米材料以及金属单原子催化剂(SACs)作为研究对象.最后,对原位同步辐射实验方法发展及其针对电化学反应动态过程的研究进行了展望,旨在通过揭示电化学反应的动态机理来指导和合成高效稳定的催化材料.

The electrochemical interface kinetics determines all electrochemical reaction properties.The multidimensional in situ observation of the dynamic process of electrochemical reaction on the interface of the electrode surface is of great significance for the design,synthesis and screening of catalyst structures in typical electrochemical energy storage technologies(electrolyzers,fuel cells),but the complex electrochemical interface and the small and rapid reaction intermediate state signal bring great challenges to the study of the dynamic process of electrochemical reaction.Synchrotron radiation Fourier transform infrared spectroscopy(SR-FTIR)has a unique molecular fingerprint recognition function,which can determine the active species at the electrochemical interface.The X-ray absorption fine structure(SR-XAFS)spectroscopy,is highly sensitive to the local atomic structure of nanomaterials and can study the electrochemical reaction process at the interface in real time.The SR-FTIR correlated spectroscopy helps guide the design of advanced electrocatalysts for efficient,high energy-density energy systems.Based on the research work of our group in recent years,this review systematically introduces how to obtain high quality experimental results of synchrotron radiation infrared correlated spectroscopies in the process of electrochemical reaction,and the research results of its application to the dynamic process of electrocatalytic reactions.The currently popular metal-organic framework(MOF)nanomaterials and metal single-atom catalysts(SACs)are selected as the research objects.Finally,the development of in situ synchrotron radiation experimental methods and the study of dynamic processes in electrochemical reactions are briefly prospected,aiming at revealing the dynamic mechanism of electrochemical reactions to guide and synthesize efficient and stable catalytic materials.