催化材料服役行为的同步辐射原位X射线研究

Operando X-ray study of service behavior of catalytic materials based on synchrotron radiation

介绍了基于同步辐射的原位X射线吸收谱、原位X射线衍射谱和原位X射线光电子能谱的基本原理及功能,重点综述了原位X射线技术在电解水催化材料服役行为动态研究中的应用进展,列举了多种典型电解水催化剂在反应条件下结构动态变化的研究实例,为实现催化材料全生命周期动态构效关系的精准构建提供了技术基础.最后,分析总结了原位X射线技术在面临复杂电化学服役环境时所遇到的问题及挑战,并提出了对先进同步辐射技术及原位X射线谱学的未来展望.

Considering the energy and environmental issues faced by human society,hydrogen has become increasingly important,and electrocatalytic water splitting is considered to be an ideal way to solve these energy issues.However,although most electrocatalysts will undergo a structural evolution when in service conditions,our understanding of the service behavior of catalysts is limited.To design highly active catalysts,operando characterization techniques must be used to study their dynamic structural evolution.Today,the development of synchrotron radiation devices has reached an important stage.Synchrotron-radiation-based X-ray characterization,which has high energy,large flux,and excellent collimation compared with the ordinary laboratory X-ray source,can capture the precise structure of catalytic materials.In this review,we present the development status of synchrotron radiation devices and the basic principles of operando X-ray absorption spectroscopy,X-ray diffraction spectroscopy,and X-ray photoelectron spectroscopy based on synchrotron radiation.In addition,we highlight studies related to the dynamic service behavior of water-splitting catalysts under real conditions and list a variety of operando studies of typical water-splitting catalysts,including NiFe hydroxide/(oxy)hydroxides,perovskite oxides,spinel oxides,and noble-metal-based catalysts.The use of operando X-ray techniques deepens our understanding of t he catalyst reaction mechanism and provides a basis for identifying the dynamic structure–performance correlation of catalysts.We summarize the problems and challenges of operando X-ray-based techniques in complex electrochemical environments and propose the prospect of an advanced synchrotron radiation facility for operando X-ray characterization.With the development of the next-generation synchrotron radiation facility,adequately using this advanced X-ray light source to study the dynamic structure–activity correlation of catalytic materials throughout their life cycle to achieve the precise design and synthesis of complex pre-catalysts will advance the development of this field by enabling greater refinement and control.