Improve the Hydrothermal Stability of Cu-SSZ-13 Zeolite Catalyst by Loading a Small Amount of Ce

热液循环 催化作用 无机化学 化学 氧化铈 沸石 离子交换 材料科学 核化学 化学工程 离子 有机化学 工程类
作者
Toyohiro Usui,Zhendong Liu,Sayoko Ibe,Jie Zhu,Chokkalingam Anand,Hirokazu Igarashi,Naoki Onaya,Yukichi Sasaki,Yuji Shiramata,Tetsuro Kusamoto,Toru Wakihara
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:8 (10): 9165-9173 被引量:123
标识
DOI:10.1021/acscatal.8b01949
摘要

Copper-ion-exchanged SSZ-13 has been demonstrated to be an effective catalyst for the ammonia selective catalytic reduction of NOx. However, the Cu-SSZ-13 is still susceptible to hydrothermal degradation, which reduces the catalyst lifetime. We herein report that the hydrothermal stability of Cu-SSZ-13 can be remarkably enhanced through loading with a small amount of cerium. To clearly reveal the enhancement effect of cerium, we focused on an aluminum-rich Cu-SSZ-13 zeolite (Si/Al ratio: 6.5) with copper loadings ranging from ca. 3.4% to 4.1%, which was found to give high hydrothermal stability while still suffering from considerable degradation upon severe hydrothermal aging. Different cerium loadings were investigated, and a cerium loading with a limited range of ca. 0.2–0.4 wt % resulted in the best enhancement. The introduction of only a small amount of cerium was beneficial because it enabled a high copper loading and abundant Brønsted acidity sites that are needed for high SCR activities over a broad temperature range. Various characterization methods, including Rietveld refinement, transmission electron microscopy with energy-dispersive X-ray spectroscopy, scanning electron microscopy, and electron-spin resonance spectroscopy revealed that the small amount of cerium ions loaded into the Cu-SSZ-13 occupied the ion-exchange sites. The appropriate amount of cerium cations at the ion-exchange sites better stabilized the framework of SSZ-13 and thus led to the enhancement effect. By contrast, excessive ion-exchange with cerium adversely affected the hydrothermal stability of the Cu-SSZ-13, resulting in degraded SCR performance.
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