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题名: Si-29 NMR and UV-Raman Investigation of Initial Oligomerization Reaction Pathways in Acid-Catalyzed Silica Sol-Gel Chemistry
作者: Depla, Anouschka1;  Lesthaeghe, David2;  van Erp, Titus S.1;  Aerts, Alexander1;  Houthoofd, Kristof1;  Fan, Fengtao3, 4;  Li, Can3, 4;  Van Speybroeck, Veronique2;  Waroquier, Michel2;  Kirschhock, Christine E. A.1;  Martens, Johan A.1
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2011-03-10
DOI: 10.1021/jp109901v
卷: 115, 期:9, 页:3562-3571
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: The initial molecular steps of the acid-catalyzed silica sol-gel process departing from tetraethylorthosilicate (TEOS) were investigated by in situ Si-29 NMR and UV-Raman spectroscopy. The use of a substoichiometric H2O:TEOS molar ratio (r-value 0.2-1.2) slowed the silicate oligomerization reaction and allowed unraveling the initial steps of silica condensation. Molecular modeling confirmed Raman signal and Si-29 NMR shift assignment. A comprehensive listing of all Raman and Si-29 NMR assignments is provided, including unique Raman assignments of cyclosilicates and the linear tetramer. The combination of experiment and modeling allowed an analysis of the reaction kinetics. The derived kinetic model and the experimental observation both revealed that the H2O:TEOS molar ratio had a strong influence on the reaction kinetics but not on the reaction pathways. The multianalytical approach led to development of an oligomerization scheme. As dominant oligomerizations, chain growth, cyclodimerization, and branching were identified. Under the investigated conditions, chains did not grow longer than pentamer, and ring sizes were limited to 6-rings. Chains of 4 Si atoms and 4-rings were abundant species. Branched rings and chains were formed by attachment of dimers and trimers. Gelation proceeded from branched 4-rings and branched chains with limited hydroxyl functionalities.
关键词[WOS]: AMORPHOUS MICROPOROUS SILICA ;  VIBRATIONAL-SPECTRA ;  CONTROLLED-RELEASE ;  FAUJASITIC ZEOLITES ;  HYDROLYSIS REACTION ;  SYNTHESIS MECHANISM ;  SI/AL RATIO ;  SPECTROSCOPY ;  FRAMEWORK ;  POLYMERIZATION
语种: 英语
WOS记录号: WOS:000287833200008
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/142418
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, B-3001 Heverlee, Belgium
2.Univ Ghent, Ctr Mol Modeling, Zwijnaarde, Belgium
3.Chinese Acad Sci, Dalian Inst Chem Phys, Sci Engn & Technol Grp, Dalian, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian, Peoples R China

Recommended Citation:
Depla, Anouschka,Lesthaeghe, David,van Erp, Titus S.,et al. Si-29 NMR and UV-Raman Investigation of Initial Oligomerization Reaction Pathways in Acid-Catalyzed Silica Sol-Gel Chemistry[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2011,115(9):3562-3571.
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