Structural and reactivity properties of Nb-MCM-41:: Comparison with that of highly dispersed Nb2O5/SiO2 catalysts

被引:134
作者
Gao, XT
Wachs, IE
Wong, MS
Ying, JY
机构
[1] Lehigh Univ, Zettlemoyer Ctr Surface Studies, Dept Chem Engn, Bethlehem, PA 18015 USA
[2] MIT, Dept Chem Engn, Cambridge, MA 02139 USA
关键词
Nb-MCM-41; Nb2O5/SiO2; catalysts; methanol oxidation; Raman spectroscopy; UV-visible diffuse reflectance spectroscopy;
D O I
10.1006/jcat.2001.3313
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 molecular structures of Nb cations in mesoporous material Nb-MCM-41 and the supported Nb2O5/SiO2 catalyst under hydrated and dehydrated conditions were investigated by in-situ Raman and UV-vis-NIR diffuse reflectance spectroscopies. Methanol oxidation was employed as a chemical probe reaction to examine reactivity/selectivity properties of these catalytic materials. The structural characterization techniques demonstrate that similar surface Nb oxide species are present in both Nb-MCM-41 and Nb2O5/SiO2 catalysts, which are sensitive to the environmental conditions (ambient or dehydrated). However, the characterization results also suggest that some Nb atoms in Nb-MCM-41 may be incorporated within the siliceous framework. The spectroscopic results revealed that under dehydrated conditions, the Nb cations in Nb-MCM-41 and 1% Nb2O5/SiO2 are predominantly composed of isolated NbO4 units, while the Nb cations in the supported Nb2O5/SiO2 catalysts possess polymerized NbOx species and/or bulk Nb2O5 with increasing Nb loading. The catalytic results indicate that the dispersed Nb cations in both types of catalysts are active redox sites for methanol oxidation and exhibit similar reactivity and selectivity properties due to the presence of Nb-O-Si bonds in their structures. (C) 2001 Academic Press.
引用
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页码:18 / 24
页数:7
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