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

被引:133
作者
Usui, Toyohiro [1 ]
Liu, Zhendong [2 ]
Ibe, Sayoko [2 ]
Zhu, Jie [2 ]
Anand, Chokkalingam [2 ]
Igarashi, Hirokazu [1 ]
Onaya, Naoki [1 ]
Sasaki, Yukichi [3 ]
Shiramata, Yuji [4 ]
Kusamoto, Tetsuro [5 ]
Wakihara, Toni [2 ]
机构
[1] IBIDEN Co Ltd, 1-1 Kitagata, Ibigawa, Gifu 5010695, Japan
[2] Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
[3] Japan Fine Ceram Ctr, Nanostruct Res Lab, Atsuta Ku, 2-4-1 Mutsuno, Nagoya, Aichi 4568587, Japan
[4] Rigaku Corp, Applicat Lab, 3-9-12 Matsubara Cho, Akishima, Tokyo 1968666, Japan
[5] Univ Tokyo, Grad Sch Sci, Dept Chem, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1130033, Japan
基金
日本学术振兴会;
关键词
NH3-SCR; SSZ-13; zeolite; cerium; hydrothermal stability; NOx removal; SUPERIOR CATALYST; THERMAL-STABILITY; SSZ-13; ZEOLITE; REDUCTION; NH3-SCR; NOX; CU/SSZ-13; CERIUM; SITES; SCR;
D O I
10.1021/acscatal.8b01949
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
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 Bronsted 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.
引用
收藏
页码:9165 / 9173
页数:17
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