铂、钯、铑单原子催化剂上烃类选择性还原氮氧化物的研究

Pt, Pd, Rh作为目前大量使用的汽车尾气脱氮氧化物催化剂价格昂贵、储量有限。单原子是金属催化剂分散度能够达到的极限状态。最近，项目申请人所在团队成功合成了首个具有较高活性和稳定性的单原子Pt催化剂，该催化剂对一氧化碳氧化反应的活性是传统纳米催化剂的2-3倍。本项目以探索资源节约型汽车尾气氮氧化物消除催化剂为目标，在已有工作的基础上设计合成一系列Pt, Pd, Rh单原子催化剂，考察它们对富氧条件下烃类选择还原氮氧化物反应的活性、选择性与稳定性并与传统纳米催化剂进行对比。通过本项目研究将揭示Pt, Pd, Rh单原子催化剂的合成规律，阐明单原子催化剂在烃类选择性还原氮氧化物反应中的独特催化性能、反应机理和动力学。本项目有望在汽车尾气氮氧化物脱除技术上取得突破性进展，对从原子水平认识贵金属催化剂表面氮氧化物选择性还原反应、提高贵金属利用效率、保护环境方面具有极为重要的理论和现实意义。

As the currently mostly used de-NOx catalysts for automibile exhaust, Pt, Pd, Rh have high price and limited reserves. "Single-atom" is the utmost state for the dispersion of noble metal catalysts. Recently, our research team successfully synthesized the first "single-atom" Pt catalyst which is highly active and stable under the reaction conditions. For CO oxidation reaction,the activity of the "single-atom" catalyst is 2-3 times of conventional nano-scale catalysts. This project aims at developping the resource-saving catalysts for the removal of nitrogen oxides from automobile exhausts. In this work, a series of Pt, Pd, Rh "singal-atom" catalysts will be prepared by the technologies deveoloped in the previous work of our group. The activities, selectivities and stabilities of these catalysts for the selective catalytic reduction of nitrogen oxide with hydrocarbons under oxygen-riched condtions will be studied and compared with those of conventional nano-scale catalysts.Base on this work, some knowledge about the preparation of single-atom catalysts will be acquired.Some unique characters of single-atom catalysts such as catalytic performance, reaction mechanism and kinetics will be disclosed.This project may get some breakthrough on the de-NOx technology for automobile exhaust treatment and has very important academic and realistic significance for the understanding of the selective reduction of nitrogen oxides with hydrocarbons over noble metal catalyst on atomic scale, increasing the efficiency of noble metal and environmental protection.