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由铂或钯促进的纳米结构钆掺杂二氧化铈:电子和表面结构及其与化学性质关系的研究。

Nanostructured, Gd-doped ceria promoted by Pt or Pd: investigation of the electronic and surface structures and relations to chemical properties.

作者信息

Borchert Holger, Borchert Yulia, Kaichev Vasiliy V, Prosvirin Igor P, Alikina Galina M, Lukashevich Anton I, Zaikovskii Vladimir I, Moroz Ella M, Paukshtis Eugenii A, Bukhtiyarov Valerii I, Sadykov Vladislav A

机构信息

Boreskov Institute of Catalysis, SB RAS, Novosibirsk, Russia, and Novosibirsk State University, Novosibirsk, Russia.

出版信息

J Phys Chem B. 2005 Nov 3;109(43):20077-86. doi: 10.1021/jp051525m.

Abstract

Nanostructured ceria doped with other rare earth elements is a good oxygen ion conductor, which gives rise to various catalytic applications such as the construction of membranes for syngas production by partial oxidation of methane. This article focuses on the Gd-doped cerium dioxides, which can be modified with Pt or Pd to enhance the reactivity of the lattice oxygen in interaction with methane. The aim of the work is the elucidation of correlations between the structural, electronic, and chemical properties of these nanomaterials. Detailed studies were performed for a series of samples with and without surface modification by noble metals using a complex combination of physicochemical methods: XRD, TEM, CH(4) TPR, XPS, SIMS, and FTIR spectroscopy of adsorbed CO. XPS and TPR data revealed that surface modification with noble metals enhances the reducibility of the doped ceria support, where the effect is more pronounced for Pd than for Pt. The formation of highly cationic Pd species due to strong metal support interactions provides a possible explanation for this behavior. Furthermore, the results obtained in the present work for the Gd-doped ceria system are compared to those obtained previously for the Pr-doped ceria system.

摘要

掺杂其他稀土元素的纳米结构二氧化铈是一种良好的氧离子导体,这使其具有各种催化应用,例如构建用于通过甲烷部分氧化生产合成气的膜。本文重点研究了掺钆二氧化铈,其可通过铂或钯进行改性,以增强晶格氧与甲烷相互作用时的反应活性。这项工作的目的是阐明这些纳米材料的结构、电子和化学性质之间的相关性。使用一系列物理化学方法的复杂组合,对一系列有和没有贵金属表面改性的样品进行了详细研究:XRD、TEM、CH(4) TPR、XPS、SIMS以及吸附CO的FTIR光谱。XPS和TPR数据表明,贵金属表面改性增强了掺杂二氧化铈载体的还原性,其中钯的效果比铂更明显。由于强烈的金属载体相互作用而形成的高阳离子态钯物种为这种行为提供了一种可能的解释。此外,将本工作中掺钆二氧化铈体系获得的结果与之前掺镨二氧化铈体系获得的结果进行了比较。

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