Bronsted/Lewis Acid Synergy in H-ZSM-5 and H-MOR Zeolites Studied by 1H and 27Al DQ-MAS Solid-State NMR Spectroscopy

被引:145
|
作者
Yu, Zhiwu [1 ,2 ]
Li, Shenhui [1 ]
Wang, Qiang [1 ]
Zheng, Anmin [1 ]
Jun, Xu [1 ]
Chen, Lei [1 ]
Deng, Feng [1 ]
机构
[1] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China
[2] Chinese Acad Sci, Grad Sch, Beijing 100029, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2011年 / 115卷 / 45期
基金
中国国家自然科学基金;
关键词
EXTRA-FRAMEWORK ALUMINUM; NUCLEAR-MAGNETIC-RESONANCE; C-13; CHEMICAL-SHIFT; DOUBLE-QUANTUM NMR; Y-ZEOLITE; THEORETICAL CALCULATION; QUADRUPOLAR NUCLEI; SHAPE SELECTIVITY; HZSM-5; ZEOLITES; HIGH-FIELD;
D O I
10.1021/jp203923z
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The spatial proximities of acid sites in dealuminated H-MOR and H-ZSM-5 zeolites have been comprehensively studied by two-dimensional H-1 and Al-27 double-quantum magic-angle spinning (DQ-MAS) NMR spectroscopy. H-1 DQ-MAS NMR revealed the detailed spatial proxirnities among Bronsted and Lewis acid sites, while Al-27 DQ-MAS NMR probed the detailed spatial proximities among various aluminum species in the dealuminated zeolites. It was found that all of the extra-framework aluminum species (EFAL, Lewis acid sites) are always in close proximity to the framework aluminum (Bronsted acid sites) in both H-MOR and H-ZSM-5 zeolites. The result from C-13 CP/MAS NMR of adsorbed acetone demonstrated that the spatial proximities between Bronsted and Lewis acid sites lead to a synergy effect that can remarkably enhance the Bronsted acid strength of the dealuminated zeolites. On the basis of these experimental results, we proposed a model to describe the Bronsted/Lewis acid synergy in the dealuminated zeolites.
引用
收藏
页码:22320 / 22327
页数:8
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