INFLUENCE OF THE CHOICE OF THE TEMPLATE ON THE SHORT-TERM AND LONG-TERM STABILITY OF SAPO-34 ZEOLITE

被引:138
作者
BRIEND, M
VOMSCHEID, R
PELTRE, MJ
MAN, PP
BARTHOMEUF, D
机构
[1] Laboratoire de Réactivité de Surface, URA 1106 CNRS, Université P. et M. Curie, 75252 Paris Cedex 05
[2] Laboratoire de Chimie des Surfaces, URA 1428 CNRS, 75252 Paris Cedex 05
关键词
D O I
10.1021/j100020a060
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
SAPO-34 (chabasite structure) is studied with regard to decomposition of the template [tetraethylammonium hydroxide (TEAOH) or morpholine] and subsequent hydration-dehydration cycles over a period of few hours up to 2 years. XRD, IR, Al-27 and Si-29 MAS NMR, and N-2 adsorption an used to characterize the related structural changes. The template decomposition results into shifts in Al-27 and Si-29 MAS NMR peaks reflecting its interaction with the framework. Hydration of the template-free materials leads at room temperature to a breaking of Si-OH-Al bonds, giving a partial loss of crystallinity and the formation of Q(1), Q(2), and Q(3) Si species (Si(OT)(n)(OH)(4-n)). Dehydration of the materials after about 1 or 2 day hydration gives reversibly the. initial crystallinity, the Si environment, and the porosity for the template-free materials. Long-term hydration, up to 2 years, shows that zeolites synthesized with morpholine as a template do not recover their full crystallinity and eventually none of their porosity. By contrast, TEAOH materials-are more stable, keeping up to 80% of the starting crystallinity and 70% of their porosity. The influence of the template is correlated to the formation, during synthesis of Si islands with TEAOH, while morpholine gives a larger part of isolated Si. This restricts in the TEAOH sample the number of Si-OH-Al bonds, i.e., of points where water attacks the framework.
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页码:8270 / 8276
页数:7
相关论文
共 32 条
  • [1] SOLID-STATE NMR OF SILICOALUMINOPHOSPHATE MOLECULAR-SIEVES AND ALUMINOPHOSPHATE MATERIALS
    BLACKWELL, CS
    PATTON, RL
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (13) : 3965 - 3970
  • [2] THERMAL AND HYDROTHERMAL STABILITY OF SAPO-5 AND SAPO-37 MOLECULAR-SIEVES
    BRIEND, M
    SHIKHOLESLAMI, A
    PELTRE, MJ
    DELAFOSSE, D
    BARTHOMEUF, D
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1989, (07): : 1361 - 1362
  • [3] THERMAL-STABILITY OF TETRAPROPYLAMMONIUM (TPA) AND TETRAMETHYLAMMONIUM (TMA) CATIONS OCCLUDED IN SAPO-37 MOLECULAR-SIEVES
    BRIEND, M
    LAMY, A
    PELTRE, MJ
    MAN, PP
    BARTHOMEUF, D
    [J]. ZEOLITES, 1993, 13 (03): : 201 - 211
  • [4] DEPENDENCE OF THE ACIDIC PROPERTIES OF SAPO-37 MOLECULAR-SIEVE ON SI CONTENT AND HEAT-TREATMENT
    BRIEND, M
    PELTRE, MJ
    LAMY, A
    MAN, PP
    BARTHOMEUF, D
    [J]. JOURNAL OF CATALYSIS, 1992, 138 (01) : 90 - 100
  • [5] BRIEND M, 1994, STUD SURF SCI CATAL, V84, P613
  • [6] CHEN J, 1994, STUD SURF SCI CATAL, V84, P1731
  • [7] COLTHUP NB, 1964, INTRO INFRARED RAMAN, P210
  • [8] SAPO-37 - THE IMPLICATIONS OF STRUCTURE FLEXIBILITY ON ACIDITY
    CORMA, A
    FORNES, V
    PEREZPARIENTE, J
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1993, (08) : 676 - 678
  • [9] SOLID-STATE TRANSFORMATION OF SAPO-37 MOLECULAR-SIEVE ABOVE 1100-K
    DEREWINSKI, M
    PELTRE, MJ
    BRIEND, M
    BARTHOMEUF, D
    MAN, PP
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1993, 89 (11): : 1823 - 1828
  • [10] CHANGES IN THE ENVIRONMENT OF SI AND AL IN SAPO-37 ZEOLITE DURING ACIDITY MEASUREMENTS
    DEREWINSKI, M
    BRIEND, M
    PELTRE, MJ
    MAN, PP
    BARTHOMEUF, D
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (51) : 13730 - 13735