脱铝丝光沸石中扭曲四配位铝的27Al 3Q MAS NMR研究

波谱学杂志 ›› 2005, Vol. 22 ›› Issue (1): 61-66.

脱铝丝光沸石中扭曲四配位铝的²⁷Al 3Q MAS NMR研究

南开大学 1.化学学院， 2.物理学院，天津 300071

收稿日期:2004-09-13 修回日期:2004-10-25 出版日期:2005-03-05 发布日期:2005-03-05
基金资助:
国家自然科学基金(29803004,20233030,20373029), 教育部高等学校骨干教师基金(GG-703-10055-1008)资助项目.

Detection of Distorted Tetrahedral-Coordinate Aluminum in Dealuminated Mordenite by ²⁷Al 3Q MAS NMR

1.Department of Chemistry, 2.Department of Physics, Nankai University, Tianjin, 300071, China

Received:2004-09-13 Revised:2004-10-25 Online:2005-03-05 Published:2005-03-05
Supported by:
国家自然科学基金(29803004,20233030,20373029), 教育部高等学校骨干教师基金(GG-703-10055-1008)资助项目.

摘要/Abstract

摘要：

用²⁷Al MAS, 3Q MAS NMR研究了脱铝的丝光沸石和无定形硅铝胶中的铝配位态，在丝光沸石中检测到归属于扭曲四配位铝（Distorted Tetrahedrally Coordinated Al, DTA）的信号，通过与无定形硅铝胶的比较，发现扭曲四配位铝的存在是活化和脱铝酸性沸石的典型特征. 从这些结果推断：DTA可能是沸石骨架脱铝形成非骨架铝的中间状态.

关键词: 核磁共振, 多量子魔角旋转核磁共振, 脱铝, 丝光沸石, 扭曲四配位铝

Abstract:

²⁷Al MAS and 3Q MAS NMR spectroscopy was applied to study the aluminum coordination in dealuminated zeolite mordenite and amorphous silica alumina. A signal ascribed to distorted tetrahedral coordinate Al (DTA) was detected. By comparison with amorphous silica alumina, it was found that the presence of distorted tetrahedral coordinate species is a typical feature in crystalline zeolites after activation and dealumination. From these experimental results we suggest that the DTA species, which are absent in amorphous silicaalumina, locate at the interface between the crystalline framework lattice and the extra-framework species formed by dealumination.

Key words: NMR, multiple quantum magic angle spinning (3Q MAS) NMR, mordenite, dealumination, distorted tetrahedral-coordinated Al (DTA)

中图分类号:

O482.53

费海龙, 孙平川, 陈铁红, 李宝会, 丁大同. 脱铝丝光沸石中扭曲四配位铝的²⁷Al 3Q MAS NMR研究[J]. 波谱学杂志, 2005, 22(1): 61-66.

FEI Hai-Long, SUN Ping-Chuan, Chen-Tie-Hong, LI Bao-Hui, DING Da-Tong. Detection of Distorted Tetrahedral-Coordinate Aluminum in Dealuminated Mordenite by ²⁷Al 3Q MAS NMR[J]. Chinese Journal of Magnetic Resonance, 2005, 22(1): 61-66.

参考文献

[1] Biaglow A I, Parillo D J, Kokotailo G T, et al. A study of deluminated faujastites
[J]. J Catal, 1994, 148: 213-223.

[2] Klinowski J. Solid-state NMR studies of molecular sive catalyst
[J]. Chem Rev, 1991, 91: 1 459-1 479.

[3] Luo Q(罗晴），Cheng M J(程谟杰）, Deng F(邓风）. Characterization of Al species in MCM-22 Zeolite by solid state NMR(用固体核磁方法研究MCM-22分子筛中的Al状态）
[J]. Chinese J Magn Reson(波谱学杂志）, 2001,18(2):238-241.

[4] Samoson A, Lippmaa E, Engelhardt G, et al. Quantative high-revolution ²⁷AlNMR:tetrahedral non framework alluminium in hydrothermally treated zeolites
[J]. Chem Phys Lett, 1987, 134: 589-592.

[5] Gilson J P, Edwards C, Peters W, et al. Penta-co-ordinated aluminium zeolites and alumino silicates
[J]. J Chem Soc, Chem Commun, 1987: 1(2), 91-92.

[6] Wang K X(王凯旋）, Guo Z Y(郭振亚）, Wang J Z(王敬中）, et al. NMR studies on dealuminated Y Zeolites(Y型沸石脱铝机制和铝状态的NMR研究）
[J]. Chinese J Magn Reson(波谱学杂志）, 1995, 12(2): 119-126.

[7] Frydman L, Harwood J S. Isotropic spectra of half-integer quadrupolar spins from bidimensional magic-angle spinning NMR
[J]. J Am Chem Soc, 1995 , 117: 5 367-5 368.

[8] Fernandez C, Amoureux J P. 2D multiquantum MAS-NMR spectroscopy of ²⁷Al in aluminophosphate molecular sieves
[J]. J Chem Phys Lett, 1995, 242 : 449-454.

[9] Chen T H, Wouters B H, Grobet P J. Aluminium coordinations in zeolite mordenite by ²⁷Al multiple quantum MAS NMR spectroscopy
[J]. Eur J Inorg Chem, 2000. 281-285.

[10] Wouters B H, Chen T H, Grobet P J. Reversible tetrahedral-octahedral framework aluminum transformation in Zeolite Y
[J]. J Am Chem Soc, 1998, 120: 11 419-11 425.

[11] Van Bokhoven J A, Koningsberger D C, Kunkeler P, et al. Stepwise dealumination of zeolite beta at specific T-Sites observed with ²⁷Al MAS and \{\}\+\{27\}Al 3Q MAS NMR
[J]. J Am Chem Soc, 2000, 122 : 12 842-12 847.

[12] Fyfe C A, Bretherton J L, Lam L Y. Solidstate NMR detection, characterization, and quantification of the multiple aluminum environments in US-Y Catalysts by ²⁷Al MAS and 3QMAS experiments at very high field
[J]. J Am Chem Soc, 2001, 123: 5 285-5 291.

[13] Gore K U, Abraham A, Hegde S G. et al. Ganapathy S. ²⁹Si and ²⁷Al MAS/3Q-MAS NMR studies of high silica USY zeolites
[J]. J Phys Chem B, 2002, 106: 6 115-6 120.

[14] Chen T. H, Guan N J, Wang J Z. Dealumination process of zeolite omega monitored by ²⁷Al 3Q/MAS NMR spectroscopy
[J]. Catal Today, 2004, 93-95C: 627-663.

[15] Weckhuysen B M, De Ridder L M, Grobet P J, et al. Redox behavior and dispersion of supported chromium catalysts
[J]. J Phys Chem, 1995, 99: 320-326.

脱铝丝光沸石中扭曲四配位铝的²⁷Al 3Q MAS NMR研究

Detection of Distorted Tetrahedral-Coordinate Aluminum in Dealuminated Mordenite by ²⁷Al 3Q MAS NMR

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