Organic-free modulation of the framework Al distribution in ZSM-5 zeolite by magnesium participated synthesis and its impact on the catalytic cracking reaction of alkanes

被引:44
作者
Chen, Kang [1 ,2 ,3 ]
Wu, Xueqiu [4 ]
Zhao, Jiyu [1 ,2 ,3 ]
Zhao, Hongjuan [5 ]
Li, Anhui [4 ]
Zhang, Qiang [1 ,2 ,3 ]
Xia, Tian [1 ,2 ,3 ]
Liu, Peng [1 ,2 ,3 ]
Meng, Bo [1 ,2 ,3 ]
Song, Weiyu [4 ]
Zhu, Xiaochun [1 ,2 ,3 ]
Liu, Honghai [5 ]
Gao, Xionghou [5 ]
Xu, Chunming [1 ,2 ,3 ]
Shen, Baojian [1 ,2 ,3 ]
机构
[1] China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
[2] China Univ Petr, Key Lab Catalysis CNPC, 18 Fuxue Rd, Beijing 102249, Peoples R China
[3] China Univ Petr, Coll Chem Engn & Environm, 18 Fuxue Rd, Beijing 102249, Peoples R China
[4] China Univ Petr, State Key Lab Heavy Oil Proc, Coll Sci, 18 Fuxue Rd, Beijing 102249, Peoples R China
[5] PetroChina Co Ltd, Petrochem Res Inst, Block A42 Sci Base PetroChina, Beijing 102206, Peoples R China
基金
中国国家自然科学基金;
关键词
Al distribution; ZSM-5; zeolite; Hydride transfer; Propylene; Catalytic cracking; TEMPERATURE-PROGRAMMED DESORPTION; RESOLUTION AL-27 NMR; ONE-POT SYNTHESIS; LEWIS-ACID SITES; SOLID-STATE NMR; AB-INITIO; MONOMOLECULAR CRACKING; PYRIDINE; OLEFINS; DEALUMINATION;
D O I
10.1016/j.jcat.2022.07.032
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
Al distribution engineering is an effective way to tune the catalytic performance of ZSM-5 zeolite. In the present work, a series of [Al, Mg]-ZSM-5 with different Mg contents were obtained by hydrothermal synthesis method. For comparison, Mg/ZSM-5 with a comparable Mg content were also prepared using the conventional impregnation method. Characterizations of XPS-sputtering, H-2-TPR and Py-IR indicated the distribution and coordination structures of Mg in the samples obtained by the two preparation methods were quite different. Besides, the introduction of magnesium by hydrothermal synthesis well regulates the location of framework Al, which is not possible by the impregnation method. Al-27 MAS NMR and UV-vis-DRS of Co2+-exchanged zeolites demonstrated [Al,1.0 Mg]-ZSM-5 has less aluminum in the channel intersections compared to conventional HZSM-5. Finally, the significantly lower content of "Al pairs" in [Al,1.0 Mg]-ZSM-5 inhibits the hydride transfer process, resulting in higher yields of propylene in noctane and crude oil catalytic cracking reactions. (C) 2022 Elsevier Inc. All rights reserved.
引用
收藏
页码:735 / 750
页数:16
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