Effects of the Topological Structure of Different Cu-Zeolites on the Relationship between Soot and NOx Removal on NH3–SCRF

烟灰 沸石 氮氧化物 催化作用 氧化还原 柴油颗粒过滤器 吸附 拓扑(电路) 选择性 材料科学 选择性催化还原 化学工程 无机化学 化学 微粒 物理化学 燃烧 有机化学 冶金 数学 组合数学 工程类
作者
Zhimu Ye,Pengcheng Zhao,Xincheng Tang,Takeshi Hagio,Katsutoshi Sato,Katsutoshi Nagaoka,Xinling Li
出处
期刊:Energy & Fuels [American Chemical Society]
卷期号:38 (3): 2212-2223 被引量:4
标识
DOI:10.1021/acs.energyfuels.3c03034
摘要

Experimental studies were carried out to explore the effect of zeolite topology on NO x purification and soot oxidation in ammonia selective catalytic reduction coated diesel particulate filter (SCRF) catalysts. The catalytic activity of Cu-exchanged zeolites Cu/SSZ-13 (CHA topology), Cu/ZSM-5 (MFI), and Cu/BEA(BEA) was evaluated in the NH 3 –SCRF. Experiments with XRD and ICP-SFMS demonstrated that the three types of samples retained their typical structural peaks after Cu modification, and the similar ratios of Cu/Al and Si/Al ensure that the primary cause of different catalytic performances was caused by different framework structures. As determined by laboratory experiments with synthetic gas, Cu/SSZ-13 exhibited an extended activity window and a higher deNO x efficiency at NO 2 /NO x below 0.5. In addition, Cu/ZSM-5 consistently exhibited superior CO 2 selectivity in soot-loading experiments, regardless of the NO 2 concentration. When loaded with soot, Cu/BEA exhibited exceptional deNO x performance at NO 2 /NO x = 0.5. NH 3 was observed to have a negative effect on soot oxidation by NO 2, while the consumption of NO 2 by soot oxidation contributed to the NO 2 –SCR reaction being aided. Influenced by different zeolite structural features, the degree of diffusion of copper in the zeolite as well as the replacement sites are different, thus forming different ratios of copper species. For instance, the presence of Z2Cu sites, which can adsorb more NH 3 molecules than ZCuOH sites as indicated by the in situ DRIFTS results, and the presence of Cu + with stronger redox properties compared to Cu 2+, can be influenced by these structural characteristics. Additionally, soot particles have the ability to act as adsorption sites for the NH 3 –SCR reaction.
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