Crystal Mechanism of Cage-Based Small-Pore Molecular Sieves: A Case Study of CHA and LEV Structures
- 주제(키워드) "Zeolite"
- 발행기관 포항공과대학교 일반대학원
- 지도교수 홍석봉
- 발행년도 2017
- 학위수여년월 2017. 2
- 학위명 석사
- 학과 및 전공 일반대학원 환경공학부
- 실제URI http://www.dcollection.net/handler/postech/000002330309
- 본문언어 영어
- 저작권 포항공과대학교 논문은 저작권에 의해 보호받습니다.
초록/요약
The elucidation of the crystallization mechanism of zeolites is one of the most important topics in zeolite science. Here we have investigated the formation pathway for CHA and LEV zeolite crystals, the aluminosilicate and silicoaluminophosphate versions, respectively, in the presence of the organic structure-directing agents (SDAs), TMAdA+, TEA+, AN, and HMI. The crystallization process was monitored using a combination of ex-situ 1H-13C CP MAS NMR and IR spectra of a series of solid products recovered as a function of time during the crystallization process. We demonstrated that in the overall crystallization mechanism of CHA and LEV zeolite, the construction of large cha- and lev-cages, with complete incorporation of organic SDAs, precedes that of the small d6r-cages in the aluminoslilicate and silicoaluminophosphate forms. Crystallization can be viewed as an initial construction of randomly distributed cha- and lev-cages at the nucleation stage. The next step is that d6r-cages are constructed by linking the tops and bottoms of the cha- and lev- cages, and finally, this linking promotes the formation and growth of CHA and LEV zeolite crystals. We also showed that the SDAs play an important role in the initial condensation and nucleation, as well as participating in the crystal growth.
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Contents
Abstract I
Contents III
List of tables V
List of figures VI
Chapter 1. Introduction 1
Chapter 2. Experimental section 13
2.1. Synthesis 13
2.1.1. Zeolite synthesis 13
2.2. Characterization 15
2.2.1. Powder X-ray diffraction 15
2.2.2. Elemental analysis 15
2.2.3. Thermal analysis 16
2.2.4. Scanning electron microscopy 16
2.2.5. Multinuclear MAS NMR spectroscopy 16
2.2.6. IR spectroscopy 17
Chapter 3. Results and discussion 18
3.1. Characterization 18
3.1.1. Powder XRD pattern and SEM image of CHA and LEV Structures 18
3.1.2. 27Al, 29Si, 31P NMR and MAS NMR spectra of CHA and LEV structures 21
3.1.3. 1H-13C MAS NMR spectra and chemical composition of CHA and LEV structures 28
3.1.4. IR spectra of CHA and LEV structures 38
3.1.5. Relative crystallinity and d6r evolution in the CHA and LEV structures 40
3.1.6. The formation pathway for CHA and LEV Structures 42
Chapter 4. Conclusions 44
Chapter 5. Summary in korean 45
Chapter 6. References 46
Acknowledgements 49
Curriculum vitae 49