Bronsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by 1H and 27Al DQ-MAS NMR Spectroscopy

被引:22
|
作者
Yu Zhiwu [1 ,2 ]
Wang Qiang [1 ]
Chen Lei [1 ]
Deng Feng [1 ]
机构
[1] Chinese Acad Sci, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Inst Phys & Math, Wuhan 430071, Hubei, Peoples R China
[2] Chinese Acad Sci, High Field Magnet Lab, Hefei 230031, Anhui, Peoples R China
基金
中国国家自然科学基金;
关键词
H-MCM-22; zeolite; dealumination; acidity; Bronsted/Lewis acid synergy; double quantum-magic angle spinning nuclear magnetic resonance; SOLID-STATE NMR; EXTRA-FRAMEWORK ALUMINUM; DEALUMINATED HY ZEOLITE; THEORETICAL CALCULATION; MCM-22; ZEOLITE; PROBE MOLECULE; HIGH-FIELD; Y-ZEOLITE; SPIN-ECHO; CATALYSTS;
D O I
10.1016/S1872-2067(10)60287-2
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Bronsted/Lewis acid sites synergy in H-MCM-22 zeolite was studied by solid-state nuclear magnetic resonance (NMR). Two-dimensional H-1 double quantum-magic angle spinning (DQ-MAS) NMR revealed the details of the spatial relationship between the Lewis and the Bronsted acid sites in a dealuminated H-MCM-22 zeolite, which implied the existence of a Bronsted/Lewis acid sites synergy. Two-dimensional Al-27 DQ-MAS NMR was used to give the details of the spatial proximities of various aluminum species. The Bronsted/Lewis acid sites synergy occurred in the supercage of the H-MCM-22 zeolite between a T-6 site Al and extra-framework Al species. C-13 CP/MAS NMR of adsorbed acetone demonstrated that the spatial proximities of the Bronsted and Lewis acid sites led to a synergy that enhanced the Bronsted acid strength of the dealuminated zeolites. H-1 MAS NMR of adsorbed deuterated pyridine confirmed that the Bronsted/Lewis acid sites synergy occurred in the supercage of H-MCM-22. This finding is important for understanding the mechanism of acid-catalyzed reactions on H-MCM-22 zeolites.
引用
收藏
页码:129 / 139
页数:11
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