期刊
Environmental Science & Technology
标题
Tandem Reaction on Ru/Cu-CHA Catalysts for Ammonia Elimination with Enhanced Activity and Selectivity
作者
Qi An, Mengyuan Zhang, Jianhua Liu, Tingxu Chen, Yueqing He, Diru Liu, Yunbo Yu, Guangyan Xu, Hong He
摘要
Ammonia emissions from vehicles and power plants cause severe environmental issues, including haze pollution and nitrogen deposition. Selective catalytic oxidation (SCO) is a promising technology for ammonia abatement, but current catalysts often struggle with insufficient activity and poor nitrogen selectivity, leading to the formation of secondary pollutants. In this study, we developed a bifunctional Ru/Cu-CHA zeolite catalyst for ammonia oxidation, incorporating both SCO sites (Ru) and selective catalytic reduction sites (SCR, Cu). Various characterizations, including HAADF-STEM, XAFS, and H2-TPR, revealed that Cu2+ cations are dispersed within the CHA zeolite, while RuOx clusters and nanoparticles are present both inside and on the surface of the zeolite. Operando DRIFTS-MS, in situ Raman spectroscopy, and DFT calculations confirmed that NH3 adsorbed on Cu2+ Lewis acid sites efficiently reduced RuO2 with a lower energy barrier, significantly enhancing the low-temperature activity of the Ru/Cu-CHA catalyst. Additionally, Cu2+ cations further facilitated the elimination of byproducts (NOx) via the tandem SCR reaction, thus greatly improving the nitrogen selectivity. This synergistic effect contributed to high catalytic activity (>94% at 200 °C) and excellent nitrogen selectivity (>90% even at high temperatures above 325 °C) for Ru2.5/Cu-CHA during practical ammonia elimination in the presence of NOx and water vapor.
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