Ru单原子、团簇和纳米晶材料的可控合成及性能研究

Noble-metal catalysts are the most widely used in industry because of their high activity, selectivity and stability for large number of important chemical reactions. Ruthenium-based catalysts are critical to many important commercial chemical processes, such as fuel cells, energy conversion, ammonia synthesis and redox reactions. Because of growth of the demand, extremely low-abundance for precious metal Ru, this is a barrier to industrial application. Therefore, improving the efficiency of Ru atom use is a key issue. Developing Ru single atom or cluster catalysts with high activity and stability might be an effective route but remain a big challenge. This project is aim to develop new synthetic method of Ru single atoms and clusters. Compared with Ru nanocrystal catalysts, we will study the catalytic performance of supported Ru single atoms and clusters catalysts through some important model reactions. This work may open up a new thought of exploring atomic-scale, stable, highly active catalysts.

贵金属由于其具有独特的催化活性、选择性和稳定性，作为一类十分重要的催化剂材料已广泛应用于多种关键的工业催化反应过程中。贵金属Ru在能源存储与转化、合成氨、氧化反应中发挥了至关重要的作用。随着Ru需求量不断上升，其资源日益短缺，价格昂贵，制约其工业化应用。因次，如何提高Ru原子利用率是催化剂制备的核心问题。发展高效、稳定的Ru单原子及团簇催化剂是解决该问题的一个有效途径。本项目拟：（1）发展负载型Ru单原子、团簇和纳米晶催化剂的合成新方法，实现Ru单原子和Ru团簇的可控合成；（2）得到Ru单原子、团簇、纳米晶催化剂，通过评价材料的催化性能，探索材料结构与催化性能之间的构效关系。本项目有助于开发新的Ru单原子、团簇及纳米晶催化剂，为更高效地实现反应的催化转化以及从原子尺度探索催化剂的构效关系提供新思路。

该项目围绕单原子、团簇、纳米晶催化材料的合成方法、结构调控与催化性能开展研究。项目的实施取得了系列重要进展：1，发展了单原子、团簇和纳米晶合成方法学；2，从原子和分子层次上深入认识了单原子、团簇与纳米晶催化剂之间的性能差异性，揭示了催化反应的活性中心；3，针对有工业应用前景的催化反应，实现了高活性高稳定性催化剂的设计。项目执行期间共发表学术论文50篇，包括Nature Chem. 1篇，Nature Nanotech. 1篇，Nature Catal. 2篇，Nature Commun.6篇，J. Am. Chem. Soc.10篇，Angew. Chem. Int. Ed.19篇，Adv. Mater.5篇，Nano Lett.5篇等。项目研究成果对于开发新的负载型单原子和团簇催化剂，更高效地实现催化转化提供了新思路。