Water-induced morphology changes in BaO/γ-Al2O3 NOx storage materials:: An FTIR, TPD, and time-resolved synchrotron XRD study

被引:35
作者
Szanyi, Janos [1 ]
Kwak, Ja Hun
Kim, Do Heui
Wang, Xianqin
Chimentao, Ricardo
Hanson, Jonathan
Epling, William S.
Peden, Charles H. F.
机构
[1] Pacific NW Natl Lab, Inst Interfacial Catalysis, Richland, WA 99352 USA
[2] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
[3] Univ Rovira & Virgili, Dept Engn Quim, Tarragona, Spain
[4] Univ Waterloo, Waterloo, ON N2L 3G1, Canada
关键词
D O I
10.1021/jp067932v
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 effect of water on the morphology of BaO/Al2O3-based NOx storage materials was investigated using Fourier transform infrared spectroscopy, temperature programmed desorption, and time-resolved synchrotron X-ray diffraction techniques. The results of this multispectroscopy study reveal that in the presence of water surface Ba-nitrates convert to bulk nitrates and water facilitates the formation of large Ba(NO3)(2) particles. The conversion of surface to bulk Ba-nitrates is completely reversible (i.e., after the removal of water from the storage material a significant fraction of the bulk nitrates reconverts to surface nitrates). NO2 exposure of a H2O-containing (wet) BaO/Al2O3 sample results in the formation of nitrites and bulk nitrates exclusively (i.e., no surface nitrates form). After further exposure to NO2, the nitrites completely convert to bulk nitrates. The amount of NOx taken up by the storage material, however, is essentially unaffected by the presence of water regardless of whether the water was dosed prior to or after NO2 exposure. On the basis of the results of this study, we are now able to explain most of the observations reported in the literature on the effect of water on NOx uptake on similar storage materials.
引用
收藏
页码:4678 / 4687
页数:10
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