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Kim, Wookdong
나노물질 및 화학반응 연구단
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Mesopore-selective incorporation of strong Brønsted acid catalytic sites via aluminium grafting on hierarchically porous siliceous MFI zeolite

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Title
Mesopore-selective incorporation of strong Brønsted acid catalytic sites via aluminium grafting on hierarchically porous siliceous MFI zeolite
Author(s)
Wookdong Kim; Jeong-Chul Kim; Seungjun Lee; Jaeheon Kim; Ryong Ryoo
Subject
Aluminum grafting, ; External acid sites, ; Hierarchical zeolites, ; Post-synthetic method
Publication Date
2020-10
Journal
MICROPOROUS AND MESOPOROUS MATERIALS, v.305, pp.110353
Publisher
ELSEVIER SCIENCE BV
Abstract
© 2020 Elsevier Inc. Post-synthetic Al grafting onto the surface silanols in mesoporous MFI zeolite has been investigated in an attempt to obtain a model catalytic material that possesses strong Brønsted acid sites at mesopore surfaces of the zeolite, but not inside the microporous framework. To this end, a siliceous MFI zeolite with a mesopore/micropore hierarchy was synthesized using a meso-micro dual structure-directing diammonium surfactant. The hierarchically porous zeolite was treated with anhydrous AlCl3 for the formation of Si–O–Al bonding with silanols on the mesopore surfaces. According to solid-state 31P NMR spectroscopy of the surface-adsorbed phosphine oxides and catalytic activity for decalin cracking, the Al-grafting treatment performed in the conventional manner resulted in the formation of weak Brønsted acid sites, similar to Al grafting on SBA-15 mesoporous silica. To obtain strong Brønsted acid sites, we have developed a method of heating the AlCl3-grafted zeolite in a controlled-humidity chamber before calcination. The resultant zeolite was catalytically active for cracking of hydrocarbons requiring strong acid sites, but not for methanol-to-hydrocarbon conversion. The results support that the moisture treatment caused a local reconstruction of the initially grafted Al–O–Si framework portion to a strong Brønsted acid site. In addition, our model catalytic zeolite material unveiled the catalytic activity of Brønsted acid sites at the mesopore surfaces in hierarchically porous zeolite in n-octane cracking. Furthermore, we confirmed that this method was effective for other mesoporous MFI zeolites obtained through a post-synthetic desilication route
URI
https://pr.ibs.re.kr/handle/8788114/7622
DOI
10.1016/j.micromeso.2020.110353
ISSN
1387-1811
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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