Study on the Performance of the Zr-Modified Cu-SSZ-13 Catalyst for Low-Temperature NH3-SCR

催化作用 选择性催化还原 X射线光电子能谱 解吸 沸石 傅里叶变换红外光谱 化学 空间速度 无机化学 分析化学(期刊) 材料科学 吸附 选择性 化学工程 物理化学 有机化学 工程类
作者
Huiyong Du,Shuo Yang,Ke Li,Qian Shen,Min Li,Xuetao Wang,Chenyang Fan
出处
期刊:ACS omega [American Chemical Society]
卷期号:7 (49): 45144-45152 被引量:15
标识
DOI:10.1021/acsomega.2c05582
摘要

Cu-SSZ-13 and Zr-modified Cu-SSZ-13 catalysts with different Zr/Cu mass ratios were prepared by ion-exchange and impregnation methods, respectively. The NH3-SCR performance tests were performed using the catalyst performance evaluation device to investigate the effects of different Zr/Cu mass ratios on the catalyst ammonia-selective catalytic reduction (NH3-SCR) performance. X-ray diffraction, ICP-OES, BET, NH3 temperature-programed desorption (NH3-TPD), H2 temperature-programmed reduction (H2-TPR), X-ray photoelectron spectrometry, and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) were used to characterize the catalysts. The results show that the prepared Cu-SSZ-13 catalyst had good catalytic activity. Zr introduction was carried out on this basis. The results showed that proper Zr doping improved the catalytic activity at low temperatures and widened the high-temperature stage, with an optimal activity stage at a Zr/Cu mass ratio of 0.2. The NO x conversion efficiency was close to 100% at 200 °C and over 80% at 450 °C. The active species were well dispersed on the catalyst surface, and the metal modification did not change the crystal structure of the zeolite. The NH3-TPD results showed that the Zr-modified catalyst had more abundant acid sites, and the H2-TPR results indicated that the Cu species on the catalyst had excellent reducibility at low temperatures. The interaction between Cu and Zr could regulate the Cu+ and Cu2+ proportion on the catalyst surface, which facilitated the increase in the Cu+ for fast SCR reaction at low temperatures. With abundant acid sites and both SCR reactions following the Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanism on the catalyst surface at a low temperature of 150 °C, more abundant acid sites and reaction paths created favorable conditions for NH3-SCR reactions at low temperatures.
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