Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Materials for Energy Conversion of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, P. R. China.
Chem Soc Rev. 2017 Apr 3;46(7):1977-2000. doi: 10.1039/c6cs00828c.
Understanding the surface chemistry of solid catalysts is of great importance for the rational design of structures of advanced catalysts; however, long-term challenges remain due to the complex and non-uniform catalyst structures and the lack of suitable characterization techniques. Surface chemistry studies of single-crystal-based model catalysts with well-defined surface structures under ultra-high vacuum conditions have been developed as one approach, but the so-called materials gap and pressure gap are sometimes encountered when the acquired understanding is extended to the industrial reaction conditions. Recently emerging uniform catalytic nanocrystals with well-defined surface structures consist of a novel type of model catalysts, whose surface chemistry can be studied under the same conditions as the industrial reaction conditions; meanwhile, the surface chemistry of powder catalysts can be studied to some extent due to the development of advanced characterization techniques. Group IB metals (Cu, Ag, Au) and related oxides constitute a class of catalysts with unique catalytic properties and wide catalytic applications. We herein review the recent progress in the surface chemistry of Group IB metals and related oxides from single-crystal-based model catalysts to nanocrystal-based model catalysts and powder catalysts in an attempt to summarize the commonalities and to discuss the differences among the surface chemistry acquired from the catalysts with different levels of complexity. The surface chemistry of Group IB metals and related oxides is compared and correlated to their catalytic performance. A concept of model catalysts from single crystals to nanocrystals is prospected for the investigation of the surface chemistry of solid catalysts to approach industrial reaction conditions as closely as possible.
理解固体催化剂的表面化学对于先进催化剂结构的合理设计至关重要;然而,由于催化剂结构复杂且不均匀,以及缺乏合适的表征技术,长期以来一直存在挑战。在超高真空条件下对具有明确表面结构的单晶基模型催化剂进行表面化学研究是一种方法,但在将所获得的认识扩展到工业反应条件时,有时会遇到所谓的材料差距和压力差距。最近出现的具有明确表面结构的均匀催化纳米晶体由一种新型的模型催化剂组成,其表面化学可以在与工业反应条件相同的条件下进行研究;同时,由于先进表征技术的发展,也可以在一定程度上研究粉末催化剂的表面化学。IB 族金属(Cu、Ag、Au)及其相关氧化物构成了一类具有独特催化性能和广泛催化应用的催化剂。本文综述了从单晶基模型催化剂到纳米晶基模型催化剂和粉末催化剂的 IB 族金属及其相关氧化物的表面化学的最新进展,试图总结它们之间的共性,并讨论从不同复杂程度的催化剂获得的表面化学之间的差异。比较了 IB 族金属及其相关氧化物的表面化学与其催化性能,并对从单晶到纳米晶的模型催化剂的概念进行了展望,以期尽可能接近工业反应条件来研究固体催化剂的表面化学。