Controlled structural collapse of high-Al zeolite via decationization and its applications in adsorption = 제올라이트의 구조 붕괴 조절에 따른 기공 구조 변화에 대한 연구 및 흡착 특성 분석

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In zeolite chemistry, it was known that the decationization ($NH4^+$ ion-exchange followed by calcination) of highly aluminous zeolites (Si/Al<1.3) results in a loss of zeolite crystallinity. Although such structural transformation has been known for several decades, the pore structures of the amorphous phases have not been investigated. The reason might be attributed to the lack of scientific interests in the ill-defined amorphous materials and to the hasty conclusion that the atomically ‘collapsed’ phase would be nonporous. In this thesis, two phenomena, generation of mesopores and reduction of micropore size, was observed via decationization of two different zeolites (FAU and LTA structures). In case of NaX zeolite (FAU structure, Si/Al = 1.2), the controlled decationization of NaX zeolite can produce hierarchically micro-/mesoporous zeolites and solely mesoporous aluminosilicates having an amorphous framework. The hierarchically porous NaX zeolite has significantly higher adsorption capacities and catalytic activities for bulky molecular species compared with conventional NaX zeolite due to the presence of secondary mesoporosity that allows the facile diffusion of bulky molecules. The controlled collapse or atomic disordering of NaA zeolite (LTA structure, Si/Al = 1.0) with decationization can systematically narrow the effective pore size below 0.4 nm and tune the molecular sieving effect. As the zeolite is gradually disordered, the adsorption amounts for all gas molecules decrease; however, larger molecules show a much faster decrease than that of the smaller ones. Consequently, the adsorption selectivities could be remarkably enhanced for various gas pairs. Moreover, the decationized NaA zeolites were applied for mixed matrix membrane (MMM) to improve their $CO_2$/$CH_4$ permselectivity by enhancing the diffusion selectivity. This simple and controllable post-modification method would be industrially suitable for generation of mesopores and control of molecular sieving effect, which are promising as adsorbents and heterogeneous catalysts.
Advisors
Choi, Minkeeresearcher최민기researcher
Description
한국과학기술원 :생명화학공학과,
Publisher
한국과학기술원
Issue Date
2018
Identifier
325007
Language
eng
Description

학위논문(박사) - 한국과학기술원 : 생명화학공학과, 2018.8,[viii, 79 p. :]

Keywords

zeolite▼adecationization▼aamorphous▼ahierarchically porous▼amolecular sieving effect; 제올라이트▼a탈양이온화▼a비결정성▼a위계다공성▼a분자체 효과

URI
http://hdl.handle.net/10203/264933
Link
http://library.kaist.ac.kr/search/detail/view.do?bibCtrlNo=827911&flag=dissertation
Appears in Collection
CBE-Theses_Ph.D.(박사논문)
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