Defective sites in ZSM-5 zeolite synthesized by n-butylamine template facilitating uniform meso-microporosity by alkali-treatment

被引:25
作者
Sun, Yu [1 ]
Ma, Tong [1 ,2 ]
Cao, Shiwei [1 ]
Wang, Jie [1 ]
Meng, Xiaoling [1 ]
Gong, Yanjun [1 ]
Zhang, Zhongdong [3 ]
Ma, An [3 ]
Liu, Ping [4 ]
机构
[1] China Univ Petr, Coll Chem Engn, Key Lab Catalysis CNPC, State Key Lab Heavy Oil Proc, Beijing, Peoples R China
[2] PetroChina Int Co Ltd, Beijing, Peoples R China
[3] PetroChina Co Ltd, Petrochem Res Inst, Beijing, Peoples R China
[4] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
ZSM-5; N-butylamine; Desilication; Uniform mesopore; Defective sites; METHANOL-TO-HYDROCARBONS; MESOPOROSITY DEVELOPMENT; CATALYTIC PERFORMANCE; FACILE SYNTHESIS; AL DISTRIBUTION; MFI ZEOLITES; DESILICATION; CONVERSION; ALUMINUM; H-ZSM-5;
D O I
10.1016/j.micromeso.2021.111360
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Two ZSM-5 zeolites (denoted as BZ and TZ series), respectively synthesized by using n-butylamine (BA) and tetrapropylammonium (TPA(+)) as template, were transformed to pertinent hierarchical zeolites (BZ-AT and TZ-AT) by post-treatment via alkali-treatment. The both ZSM-5 zeolites have distinct defective sites, which are crucial importance for their properties in terms of forming meso-microporosity and performance in the methanol to olefin reaction. By alkali treating ZSM-5 zeolites (BZ-80 and TZ-80) with comparable SiO2/Al2O3 of 80, the hierarchical zeolite BZ-80-AT proves higher Desilication Efficiency than TZ-80-AT. Notably, BZ-80-AT features a uniform distributed meso-microporosity with mesopore size centered around 10 nm, larger external surface area and mesopore volume, while TZ-80-AT displays a centrally hollow structure with cavity size of more than 200 nm in diameter. Characterization results demonstrate more silanol nests in BZ-80, facilitating uniform desilication to create uniform mesopore in BZ-80-AT crystals. In contrast, the more internal silanols in TZ-80, along with the connatural distorted framework aluminium generate the hollowed structure in TZ-80-AT. Much should be owed to its specific micro/mesoporosity rendering better diffusivity, BZ-80-AT exhibits higher propylene and butylene selectivity as well as longer lifetime in the MTP reaction.
引用
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页数:9
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