INTERACTION BETWEEN AMMONIUM HEPTAMOLYBDATE AND NH(4)ZSM-5 ZEOLITE - THE LOCATION OF MO SPECIES AND THE ACIDITY OF MO/HZSM-5

被引:93
作者
XU, YD
SHU, YY
LIU, ST
HUANG, JS
GUO, XX
机构
[1] State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023
基金
美国国家航空航天局;
关键词
MO/HZSM-5; NH(4)ZSM-5; ZEOLITE; BRONSTED ACID SITES; METHANE ACTIVATION;
D O I
10.1007/BF00807179
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
Mo/HZSM-5 catalysts show high reactivity and selectivity in the activation of methane without using oxidants. Mo/HZSM-5 catalysts with Mo loading ranging from 0 to 10% were prepared by impregnation with an aqueous solution of ammonium heptamolybdate (AHM). The samples were dried at 393 K, and then calcined at different temperatures for 4 h. The interaction between Mo species and NH(4)ZSM-5 zeolite was characterized by FT-IR spectroscopy, differential thermal analysis (DTA) and temperature programmed decomposition (TPDE) and NH3-TPD at different stages of catalyst preparation. The results showed that if Mo/HZSM-5 catalysts were calcined at a proper temperature, the Mo species will interact with acid sites (mainly with Bronsted acid sites) and part of the Mo species will move into the channel. The Mo species in the form of small MoO3 crystallites residing on the external surface and/or in the channel, and interacting with Bronsted acid sites may be responsible for the methane activation. Strong interaction between Mo species and the skeleton of HZSM-5 will occur if the catalyst is calcined at 973 K. This may lead to the formation of MoO42- species, which is detrimental to methane activation.
引用
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页码:233 / 243
页数:11
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