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Gold supported on ceria doped by Me3+ (Me = Al and Sm) for water gas shift reaction: Influence of dopant and preparation method

机译:Me3 +(Me = Al和Sm)掺杂二氧化铈负载金对水煤气变换反应的影响:掺杂剂的影响及制备方法

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摘要

Gold catalysts supported on ceria doped by Sm and Al were studied. The influence of the preparation method, as well as the nature of dopants on the structure, properties and WGS activity are investigated. The applied methods of preparation cause the modification of ceria in a different extent. In the sample prepared by co-precipitation (CP) and doped by Al, the vacancies are located within the bulk of ceria structure, whereas in the corresponding AuCeSmCP sample the vacancies are located most likely around Sm and the ceria structure seems to be better ordered than the Al doped ceria. There is no distinct correlation between the reducibility and WGS activity of the studied catalysts. The Au 4f XPS spectra of fresh samples reveal higher contribution of dispersed form of Au for Sm doped catalysts than for the corresponding Al doped samples. The Ce 3d XPS spectra disclose also a higher concentration of Ce3+ evaluated before the catalytic operation for Sm doped catalysts as compared with the Al doped fresh samples. The observations by "in situ" FT-IR spectroscopy agree well with the model of active sites and the, mechanism of the WGS reaction proposed recently by some of us. The amount of formate species observed on the AuCeSmCP is higher than that on the AuCeAlCP catalyst and parallels the catalytic activity. The higher concentration of active sites on the surface of the AuCeSmCP catalyst facilitates the dissociation of water. © 2010 Elsevier B.V. All rights reserved.
机译:研究了Sm和Al掺杂负载在二氧化铈上的金催化剂。研究了制备方法的影响以及掺杂剂的性质对结构,性能和WGS活性的影响。所采用的制备方法在不同程度上引起二氧化铈的修饰。在通过共沉淀(CP)制备并掺Al的样品中,空位位于大部分二氧化铈结构内,而在相应的AuCeSmCP样品中,空位最可能位于Sm附近,并且二氧化铈结构似乎有序比掺铝的二氧化铈。研究的催化剂的还原性和WGS活性之间没有明显的相关性。新鲜样品的Au 4f XPS光谱显示,Sm掺杂催化剂的Au分散形式的贡献比相应的Al掺杂样品更高。 Ce 3d XPS光谱还显示,与掺Al的新鲜样品相比,掺Sm的催化剂在催化操作之前评估的Ce3 +浓度更高。 “原位” FT-IR光谱的观察结果与活性位点的模型以及我们中一些人最近提出的WGS反应的机理非常吻合。在AuCeSmCP上观察到的甲酸种类的数量高于在AuCeAlCP催化剂上发现的甲酸种类的数量,并且与催化活性平行。 AuCeSmCP催化剂表面上较高的活性位点浓度促进了水的离解。 ©2010 Elsevier B.V.保留所有权利。

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