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Pt/CeO(2)-ZrO(2) 存在于 SBA-15 的中孔内——一种更好的 CO 氧化催化剂。

Pt/CeO(2)-ZrO(2) present in the mesopores of SBA-15--a better catalyst for CO oxidation.

机构信息

Institute of Industrial Science, The University of Tokyo, Komaba 4-6-1, Meguro, Tokyo 153-8505, Japan.

出版信息

Phys Chem Chem Phys. 2010 Jul 21;12(27):7513-20. doi: 10.1039/b922046a. Epub 2010 Jun 3.

Abstract

Platinum loaded CeO(2)-ZrO(2)/SBA-15 composite material catalyzes CO oxidation at lower temperatures (<100 degrees C) than conventionally prepared Pt/CeO(2)-ZrO(2) (>150 degrees C). A sequence of reduction and reoxidation of CeO(2)- and ZrO(2)-loaded samples promotes the formation of CeO(2)-ZrO(2) solid solution on the siliceous surface as indicated by wide-angle X-ray diffraction (XRD) patterns. Furthermore, initial coating of ZrO(2) on the silica walls is quite important before CeO(2)-ZrO(2) loading in order to obtain the CeO(2)-ZrO(2) solid solution. The presence of CeO(2)-ZrO(2) particles inside the mesopores is confirmed by N(2) adsorption, low-angle X-ray diffraction, and scanning transmission electron microscopy (STEM) images. The solid solution of CeO(2)-ZrO(2) in the confined mesoporous space forms more Ce(3+) centers associated with oxygen vacancies on the surface due to the smaller size of the dispersed particles and these Ce(3+) centers are believed to be responsible for the higher catalytic activity.

摘要

负载铂的 CeO(2)-ZrO(2)/SBA-15 复合材料在比传统制备的 Pt/CeO(2)-ZrO(2)(>150°C)更低的温度(<100°C)下催化 CO 氧化。CeO(2)-和 ZrO(2)负载样品的还原和再氧化序列表明,在硅质表面上形成了 CeO(2)-ZrO(2)固溶体,这一点可以通过广角 X 射线衍射(XRD)图谱得到证实。此外,在负载 CeO(2)-ZrO(2)之前,ZrO(2)在二氧化硅壁上的初始涂层对于获得 CeO(2)-ZrO(2)固溶体是非常重要的。通过 N(2)吸附、低角度 X 射线衍射和扫描透射电子显微镜(STEM)图像证实了介孔内 CeO(2)-ZrO(2)颗粒的存在。由于分散颗粒的尺寸较小,CeO(2)-ZrO(2)在受限介孔空间中的固溶体形成了更多与表面氧空位相关的 Ce(3+)中心,这些 Ce(3+)中心被认为是更高催化活性的原因。

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