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Ru(0001)模型催化剂在氧化和还原反应条件下:原位高压表面X射线衍射研究

Ru(0001) model catalyst under oxidizing and reducing reaction conditions: in-situ high-pressure surface X-ray diffraction study.

作者信息

He Y B, Knapp M, Lundgren E, Over H

机构信息

Department of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring, D-35392 Giessen, Germany.

出版信息

J Phys Chem B. 2005 Nov 24;109(46):21825-30. doi: 10.1021/jp0538520.

Abstract

With surface X-ray diffraction (SXRD) using a high-pressure reaction chamber we investigated in-situ the oxidation of the Ru(0001) model catalyst under various reaction conditions, starting from a strongly oxidizing environment to reaction conditions typical for CO oxidation. With a mixture of O(2) and CO (stoichiometry, 2:1) the partial pressure of oxygen has to be increased to 20 mbar to form the catalytically active RuO(2)(110) oxide film, while in pure oxygen environment a pressure of 10(-5) mbar is already sufficient to oxidize the Ru(0001) surface. For preparation temperatures in the range of 550-630 K a self-limiting RuO(2)(110) film is produced with a thickness of 1.6 nm. The RuO(2)(110) film grows self-acceleratedly after an induction period. The RuO(2) films on Ru(0001) can readily be reduced by H(2) and CO exposures at 415 K, without an induction period.

摘要

利用配备高压反应腔的表面X射线衍射(SXRD)技术,我们在各种反应条件下对Ru(0001)模型催化剂的氧化过程进行了原位研究,反应条件从强氧化环境到典型的CO氧化反应条件。在O₂和CO的混合物(化学计量比为2:1)中,氧气的分压必须增加到20毫巴才能形成具有催化活性的RuO₂(110)氧化膜,而在纯氧环境中,10⁻⁵毫巴的压力就足以氧化Ru(0001)表面。对于550 - 630 K范围内的制备温度,会生成厚度为1.6纳米的自限性RuO₂(110)膜。RuO₂(110)膜在经过诱导期后会自加速生长。Ru(0001)上的RuO₂膜在415 K下通过暴露于H₂和CO可很容易地被还原,且无诱导期。

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