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Synthesis and Structural Analysis of High-Silica ERI Zeolite with Spatially-Biased Al Distribution as a Promising NH3-SCR Catalyst
被引:5
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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