Journal of Physical Chemistry, Vol.98, No.40, 10216-10224, 1994
SAPO-18 Catalysts and Their Bronsted Acid Sites
The incorporation of silicon via direct synthesis into AlPO4-18 (AET), which has a framework structure related to, but crystallographically distinct from, that of the well-known solid acid catalyst SAPO-34, was investigated by a range of techniques. Unlike the Si/(Si + Al + P) ratio (typically about 0.10) in SAPO-34, which can be varied only within a very narrow range under normal synthetic conditions, the Si/(Si + Al + P) ratio in SAPO-18 is tunable from 0 to 0.10 by varying the silicon content in the synthetic gel. Si-29 MAS NMR spectroscopy reveals that silicon substitutes for both phosphorus and aluminum in SAPO-18, whereas in SAPO-34, silicon substitutes only for phosphorus. Infrared and H-1 MAS NMR spectroscopies and temperature-programmed desorption (TPD) of ammonia were used to examine the Bronsted acid sites borne by SAPO-18 samples. As expected, the concentration of Bronsted acid sites in all SAPO-18 samples is much less than that in SAPO-34. In contrast to the essentially neutral AlPO4-18, which catalyzes methanol conversion only to dimethyl ether, SAPO-18 catalytically converts methanol to light olefins with high activity and selectivity. The maximum conversion of methanol to ethene and propene reaches 80% with a 100% conversion of methanol to hydrocarbons. With an optimum framework composition, SAPO-18 retains its catalytic activity and selectivity longer than SAPO-34.
Keywords:NICKEL SILICOALUMINOPHOSPHATE CATALYST;ALUMINOPHOSPHATE MOLECULAR-SIEVES;CRYSTALLINE INORGANIC SOLIDS;ANGLE-SPINNING NMR;MAS-NMR;SILICON INCORPORATION;METHANOL;CONVERSION;ZEOLITES;HYDROCARBONS