Partial transformation of MCM-41 material into zeolites: Formation of nanosized MFI type crystallites

被引:106
作者
Verhoef, MJ
Kooyman, PJ
van der Waal, JC
Rigutto, MS
Peters, JA
van Bekkum, H
机构
[1] Delft Univ Technol, Dept Appl Organ Chem & Catalysis, NL-2628 BL Delft, Netherlands
[2] Natl Ctr High Resolut Electron Microscopy, NL-2628 AL Delft, Netherlands
[3] Shell Global Solut Int, NL-1030 BN Amsterdam, Netherlands
关键词
D O I
10.1021/cm001127q
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
A new potentially catalytic material has been developed by partial recrystallization of the porewall of MCM-41. Recrystallization is induced by impregnation of MCM-41 with tetrapropylammonium hydroxide followed by a hydrothermal treatment. This procedure resulted in the formation of small particles of approximately 3 nm, which can be observed with TEM. The fact that the formation of these particles resembles the first stages of ZSM-5 formation and the fact that a templating material is used, which is also frequently applied in the synthesis of ZSM-5, suggest that the 3 nm particles have a ZSM-5 structure. Furthermore, C-13 NMR on recrystallized MCM41 shows a split-up of the methyl signal of TPA, which is also known to be present in as-synthesized ZSM-5. After calcination of the recrystallized material the small crystallites could no longer be observed, although IR measurements show still some ZSM-5-like acidity to be present. Other, milder calcination routes should be developed in order to preserve the ZSM-5 crystallites. Another stability problem encountered concerns the stability of the MCM-41 since the hydrothermal treatment severely damaged the framework. It was found that the use of a template molecule, hexadecylamine, to support the framework during the recrystallization was beneficial.
引用
收藏
页码:683 / 687
页数:5
相关论文
共 30 条
[1]  
BARRER RM, 1982, HYDROTHERMAL CHEM ZE, P174
[2]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[3]  
Blauwhoff P.M. M., 1999, CATALYSIS ZEOLITES F, VHeidelberg, P437
[4]  
Borghard W. S., 1993, Aromatics Saturation With Catalysts Comprising Crystalline Ultra-Large Pore Oxide Materials, Patent No. [US5264641, 5366945]
[5]   MECHANISM OF STRUCTURE DIRECTION IN THE SYNTHESIS OF SI-ZSM-5 - AN INVESTIGATION BY INTERMOLECULAR H-1-SI-29 CP MAS NMR [J].
BURKETT, SL ;
DAVIS, ME .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (17) :4647-4653
[6]   Methylamines synthesis: A review [J].
Corbin, DR ;
Schwarz, S ;
Sonnichsen, GC .
CATALYSIS TODAY, 1997, 37 (02) :71-102
[7]  
Corma A, 1998, STUD SURF SCI CATAL, V117, P201
[8]   In situ observation of nucleation and crystal growth in zeolite synthesis. A small-angle X-ray scattering investigation on Si-TPA-MFI [J].
de Moor, PPEA ;
Beelen, TPM ;
van Santen, RA .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (10) :1639-1650
[9]   HETEROGENEOUS ACID-CATALYZED AMINATION OF ISOBUTENE TO TERT-BUTYLAMINE [J].
DEEBA, M ;
FORD, ME .
JOURNAL OF ORGANIC CHEMISTRY, 1988, 53 (19) :4594-4596
[10]   Research and development of zeolite catalysis in the 80ties and in the 90ties as well as forthcoming trends [J].
Hoelderich, WF ;
Heinz, D .
RESEARCH ON CHEMICAL INTERMEDIATES, 1998, 24 (03) :337-348