The inorganic chemistry of guest-mediated zeolite crystallization: a comparison of the use of boron and aluminum as lattice-substituting components in the presence of a single guest molecule during zeolite synthesis

被引:30
作者
Zones, SI [1 ]
Hwang, SJ
机构
[1] ChevronTexaco Energy Res & Technol Ctr, Richmond, CA 94802 USA
[2] CALTECH, Dept Chem Engn, Pasadena, CA 91125 USA
基金
美国国家科学基金会;
关键词
zeolite synthesis kinetics; borosilicate vs. alummosilicate; SSZ-42; beta; NMR;
D O I
10.1016/S1387-1811(02)00653-4
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A comparison of two zeolite systems was made with trivalent element substitution for the use of N-benzyl-DABCO as the structure-directing agent (SDA). Boron and aluminum were used at the same initial concentrations. One reason for the study was awareness that a higher number of new zeolite structures are being found when researching borosilicate reaction mixtures. The borosilicate system studied produces SSZ-42 (IFR) while the aluminosilicate system yields beta zeolite (BEA). We focused on comparisons of the kinetics and found that the borosilicate system crystallized more rapidly, kept most of the boron in solution before incorporation into the crystal, and added mass even at the point where all solids were crystalline. In contrast, the aluminosilicate gel remained almost entirely in the solid phase through a long induction period and the mass of solids was relatively constant. The kinetics were followed by using a variety of techniques including powder XRD, pH changes, elemental analyses, partitioning in centrifugation and effects of dilution. The reaction systems were followed via NMR techniques. The transformation to crystalline could be seen by NMR for both the aluminosilicate and borosilicate reactions. Proton NMR changes were followed for both sets of solids. In addition, a profile for removal of boron from solution and towards the growing SSZ-42 was quantified by NMR. An unusual tetrahedral doublet for B-11 was found in the SSZ-42 product. No such doublet was observed for tetrahedral aluminum in the case of beta zeolite formation. (C) 2003 Elsevier Science Inc. All rights reserved.
引用
收藏
页码:263 / 277
页数:15
相关论文
共 42 条
[1]  
ABSIHALABI A, 1997, HYDROCARBON PROC FEB, P45
[2]  
Anderson M. W., 1999, 12 INT ZEOL C P MAT, P1487
[3]   Structure of ITQ-4, a new pure silica polymorph containing large pores and a large void volume [J].
Barrett, PA ;
Camblor, MA ;
Corma, A ;
Jones, RH ;
Villaescusa, LA .
CHEMISTRY OF MATERIALS, 1997, 9 (08) :1713-&
[4]   Narratives and lives: Women's health politics and the diagnosis of cancer for DES daughters [J].
Bell, SE .
NARRATIVE INQUIRY, 1999, 9 (02) :347-389
[5]   SYNTHESIS AND COMPARATIVE CHARACTERIZATION OF AL, B, GA, AND FE CONTAINING NU-1-TYPE ZEOLITIC FRAMEWORK [J].
BELLUSSI, G ;
MILLINI, R ;
CARATI, A ;
MADDINELLI, G ;
GERVASINI, A .
ZEOLITES, 1990, 10 (07) :642-649
[6]  
Chen CY, 1998, CHEM-EUR J, V4, P1312, DOI 10.1002/(SICI)1521-3765(19980710)4:7<1312::AID-CHEM1312>3.0.CO
[7]  
2-K
[8]  
CHEN CY, 2001, SURFACE SCI CATALYSI, V135
[9]  
Davis ME, 1997, CHEM IND-SER, V69, P1
[10]   ON THE INCORPORATION MECHANISM OF B AND AL IN MFI-TYPE ZEOLITE FRAMEWORKS [J].
DERUITER, R ;
JANSEN, JC ;
VANBEKKUM, H .
ZEOLITES, 1992, 12 (01) :56-62