氮氧化物
催化作用
化学
双金属片
X射线光电子能谱
吸附
共沉淀
选择性催化还原
漫反射红外傅里叶变换
反应机理
拉曼光谱
分解
红外光谱学
原位
密度泛函理论
无机化学
物理化学
化学工程
计算化学
光催化
有机化学
物理
光学
工程类
燃烧
作者
Shiwang Han,Chengbo Xuan,Luyuan Wang,Xingyu Zhang,Rong‐Guang Shao,Xingxing Cheng,Zhiqiang Wang
出处
期刊:Energy & Fuels
[American Chemical Society]
日期:2023-10-19
卷期号:37 (21): 16701-16715
被引量:2
标识
DOI:10.1021/acs.energyfuels.3c02633
摘要
In this study, Mn–Co bimetallic catalysts were prepared by a coprecipitation method. The effect of different Mn/Co molar ratios on the performance of NH3–SCR, CO-SCR, and CO oxidation was investigated, and a representative catalyst was selected to test the NOx catalytic activity of the NH3–CO-SCR synergy reaction. The microphysical and chemical properties of the samples were characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, and other analytical techniques. The CO-assisted NH3 removal mechanism of NOx was explored through in situ diffuse reflectance infrared spectroscopy (DRIFTS) and density functional theory (DFT). The results show that MC-3 has the best NOx catalytic activity and a wider SCR reaction temperature window. In the synergy reaction, the NOx conversion rate of NH3–SCR can be reached at NH3 = 400 ppm, and the N2 selectivity is effectively improved. In situ DRIFTS and DFT results show that NH3–SCR follows the L-H mechanism. In the presence of CO, some CO competes with NH3 for adsorption on the Mn sites, which suppresses the adsorption activation of NH3 and reduces the CO oxidation activity. Second, with CO participation, the activation energy required for NH4NO3* to form is lower, which promotes its further decomposition into N2 and H2O, and is of great significance for CO-assisted NH3 removal of NOx technology.
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