SAPO-18 CATALYSTS AND THEIR BRONSTED ACID SITES

被引:140
作者
CHEN, JS
WRIGHT, PA
THOMAS, JM
NATARAJAN, S
MARCHESE, L
BRADLEY, SM
SANKAR, G
CATLOW, CRA
GAIBOYES, PL
TOWNSEND, RP
LOK, CM
机构
[1] UCL ROYAL INST GREAT BRITAIN, DAVY FARADAY RES LAB, LONDON W1X 4BS, ENGLAND
[2] DUPONT CO INC, CENT RES & DEV, EXPTL STN, WILMINGTON, DE 19880 USA
[3] UNILEVER RES PORT SUNLIGHT LAB, WIRRAL L63 3JW, MERSEYSIDE, ENGLAND
基金
欧盟地平线“2020”;
关键词
D O I
10.1021/j100091a042
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
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.
引用
收藏
页码:10216 / 10224
页数:9
相关论文
共 46 条