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The isomorphous substitution of Si(4Al) with P in FAU zeolite and its stabilization effect.

Authors :
Zhang, Qiang
Zhao, Hongjuan
Liu, Xingyu
Li, Rui
Xia, Tian
Ma, Yue
Wang, Yuren
Chen, Kang
Wang, Jiujiang
Zeng, Penghui
Liu, Honghai
Liu, Chaowei
Gao, Xionghou
Xu, Chunming
Shen, Baojian
Source :
Chemical Engineering Journal. Apr2024, Vol. 486, pN.PAG-N.PAG. 1p.
Publication Year :
2024

Abstract

• A process to make P containing Y zeolite more stable. • P is incorporated into the framework by P for Si(4Al) isomorphous substitution. • Si(4Al) becomes the more stable site P(4Al) in the Y zeolite framework. • The P species in DPY zeolite are more difficult to loss than usual P modify. • The distribution of P species in DPY zeolite is more uniform. It's a dream to make zeolites more stable so as to keep the activity and stability of the catalyst. Phosphorus modification is an effective method, however, the known post-modification predominantly presents as non-framework P, and the P-loss is a big trouble in application. We have discovered that in the reaction of PCl 3 or SiCl 4 + PCl 3 with NaY zeolite, a portion of P enters the framework of the zeolite, forming a PO 4 -AlO 4 structure. Further investigations revealed that P cannot be incorporated into the framework through P for Al isomorphous substitution, but rather through isomorphous substitution with Si(4Al). PCl 3 exhibits two effects in reaction: at lower quantities, it mainly undergoes isomorphous substitution with Si(4Al); at higher quantities, it leads to zeolite dealumination generating aluminum vacancies, which disrupt the zeolite framework or promotes Si for Al isomorphous substitution. After hydrothermal aging at 800 °C for 4 h, the stable presence of framework PO 4 -AlO 4 implies that the weakest site Si(4Al) becomes the more stable site P(4Al) in the Y zeolite framework. Compared with the JPY (prepared by impregnating (NH 4) 2 HPO 4 solution to high silica Y zeolite) sample, after 10 cycles of hydrothermal and water washing treatment, the P 2 O 5 loss rate of DPY (prepared by SiCl 4 + PCl 3 with NaY) zeolite ranged from 0.4 % to 3.5 %, significantly lower compared to the range of 18.7 % to 25.9 % observed in the JPY sample. This indicates that in DPY zeolite, the interaction between P and the zeolite is stronger and less prone to loss. Moreover, P is more uniformly distributed on the surface and bulk phase of DPY than JPY sample. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
13858947
Volume :
486
Database :
Academic Search Index
Journal :
Chemical Engineering Journal
Publication Type :
Academic Journal
Accession number :
176501595
Full Text :
https://doi.org/10.1016/j.cej.2024.150422