Synthesis and Structural Analysis of High-Silica ERI Zeolite with Spatially-Biased Al Distribution as a Promising NH3-SCR Catalyst

被引:4
|
作者
Zhu, Jie [1 ]
Muraoka, Koki [1 ]
Ohnishi, Takeshi [2 ]
Yanaba, Yutaka [2 ]
Ogura, Masaru [2 ]
Nakayama, Akira [1 ]
Wakihara, Toru [1 ,3 ]
Liu, Zhendong [1 ,3 ,4 ]
Okubo, Tatsuya [1 ]
机构
[1] Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo,Bunkyo Ku, Tokyo 1138656, Japan
[2] Univ Tokyo, Inst Ind Sci, Meguro Ku, 4-6-1 Komaba,Meguro Ku, Tokyo 1538505, Japan
[3] Univ Tokyo, Inst Engn Innovat, Bunkyo Ku, 2-11-16 Yayoi,Bunkyo Ku, Tokyo 1138656, Japan
[4] Tsinghua Univ, Dept Chem Engn, State Key Lab Chem Engn, Beijing 100084, Peoples R China
基金
日本学术振兴会; 中国国家自然科学基金;
关键词
density functional calculations; high-silica ERI zeolite; NH3-SCR catalyst; NMR spectroscopy; spatially-biased Al distribution; CRYSTAL-STRUCTURE; SI-29; NMR; HYDROTHERMAL STABILITY; LTA ZEOLITES; SI/AL RATIO; ERIONITE-K; OFFRETITE; NOX; REDUCTION;
D O I
10.1002/advs.202307674
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Erionite (ERI) zeolite has recently attracted considerable attention for its application prospect in the selective catalytic reduction of NOx with NH3 (NH3-SCR), provided that the high-silica (Si/Al > 5.5) analog with improved hydrothermal stability can be facilely synthesized. In this work, ERI zeolites with different Si/Al ratios (4.6, 6.4, and 9.1) are synthesized through an ultrafast route, and in particular, a high-silica ERI zeolite with a Si/Al ratio of 9.1 is obtained by using faujasite (FAU) as a starting material. The solid-state 29Si MAS NMR spectroscopic study in combination with a computational simulation allows for figuring out the atomic configurations of the Al species in the three ERI zeolites. It is revealed that the ERI zeolite with the highest Si/Al ratio (ERI-9.1, where the number indicates the Si/Al ratio) exhibits a biased Al occupancy at T1 site, which is possibly due to the presence of a higher fraction of the residual potassium cations in the can cages. In contrast, the Al siting in ERI-4.6 and ERI-6.4 proves to be relatively random.
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页数:8
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