铁基氧化物团簇催化CO还原NO反应模拟  

Simulation of iron-based oxide cluster catalyzed CO reduction to NO reaction

作　　者：刘众元 孔繁宇 陈琳[2] 梁五洲 刘志兵 高义斌 LIU Zhong-Yuan;KONG Fan-Yu;CHEN Lin;LIANG Wu-Zhou;LIU Zhi-Bing;GAO Yi-Bing(State Grid Shanxi Electric Power Research Institute,Taiyuan 030001,China;Taiyuan University of Technolog,Taiyuan 030024,China)

机构地区：[1]国网山西省电力公司电力科学研究院,太原030001 [2]太原理工大学,太原030024

出　　处：《原子与分子物理学报》2025年第6期22-30,共9页Journal of Atomic and Molecular Physics

基　　金：国网山西省电力公司科技项目(52053023001Q);山西省科技重大专项项目(202201090301001)。

摘　　要：固定床实验表明,在深度欠氧的条件下,铁基氧化物对CO还原NO的反应具有催化作用.为进一步理解脱销催化反应机理,本文利用量化软件Gaussian模拟了铁及其三种不同价态氧化物团簇:Fe_(2)团簇、Fe_(2)O_(2)团簇、Fe_(2)O_(3)团簇催化CO还原NO的反应路径,为进一步改进脱硝反应提供理论基础.本文分析了反应过程的各阶段能量壁垒,三种团簇中最容易发生催化反应的团簇为Fe_(2),整个反应过程中的决速步为NO在Fe_(2)团簇上的解离吸附过程.Fixed-bed experiments show that iron-based oxides catalyze the reaction of CO reduction of NO under deeply underoxygenated conditions.To further understand the catalytic reaction mechanism,this paper uses the quantitative software Gaussian to simulate the reaction paths of CO reduction of NO catalyzed by iron and its three different valence oxides clusters:Fe_(2)clusters,Fe_(2)O_(2)clusters,and Fe_(2)O 3 clusters,which provides a theoretical basis for further improvement of denitrification reaction.We also analyzed the energy barriers at each stage of the reaction process,and found that the most easily catalyzed cluster among the three clusters is Fe_(2),and the decisive step in the whole reaction process is the dissociation and adsorption process of NO on Fe_(2)clusters.

关 键 词：铁团簇 脱硝 模拟 反应机理 

分 类 号：O562[理学—原子与分子物理]