CO_(2)还原铜基电催化剂的原位重构效应研究进展

Progress of in situ Reconstruction of Copper-Based Electrocatalysts in Electrochemical CO_(2) Reduction

催化过程中活性位的结构和作用机制是催化研究的核心问题。虽然Cu基催化剂在电化学CO_(2)还原反应(CO_(2)RR)中表现了较高的活性和选择性,能够生成多碳产物,但催化剂容易发生表面重构,给确定活性位结构、揭示催化机理的研究带来极大挑战,制约了反应性能的进一步提升。近年来,随着原位表征技术的发展,研究工作逐步深化认识Cu催化剂的表面重构规律,并结合理论计算阐述了基于重构后表/界面结构的催化机制,为设计开发高效催化剂提供了理论和方法基础。本综述总结CO_(2)RR中Cu基电催化剂重构效应的研究进展,讨论了不同原位表征方法在研究催化剂重构中的应用,并对催化剂的进一步设计和优化研究提出了展望。

Identifying the structure and working mechanism of active sites during catalytic processes is the key issue of catalysis research. Although Cu-based electrocatalysts exhibit high activity and selectivity in electrochemical CO_(2)reduction reaction(CO_(2)RR), especially in terms of multi-carbon products, they are prone to surface reconstruction, which brings great challenge to confirming the real structure of the active sites and unravelling the catalytic mechanism, therefore restricts the further improvement of performance. With the developments of in-situ and operando techniques, the reconstructions of Cu-based catalyst surface during CO_(2)RR have been recently unravelled experimentally, and taken into account for interpreting catalytic mechanism on restructured surface/interfaces, which provide guidelines for designing and exploiting high-performance catalysts. This review summarizes the recent progresses in the reconstruction of Cu-based electrocatalysts during CO_(2)RR, discusses the application of different in situ characterizations, and further gives a prospect on the further research.