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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Combined TPRx, in situ GISAXS and GIXAS studies of model semiconductor-supported platinum catalysts in the hydrogenation of ethene
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Combined TPRx, in situ GISAXS and GIXAS studies of model semiconductor-supported platinum catalysts in the hydrogenation of ethene

机译:结合TPRx,原位GISAXS和GIXAS研究乙烯加氢中模型半导体支撑的铂催化剂

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摘要

The preparation, characterization and catalytic reactivity of a GaN supported Pt catalyst in the hydrogenation of ethene are presented in this feature article, highlighting the use of in situ characterization of the material properties during sample handling and catalysis by combining temperature programmed reaction with in situ grazing incidence small-angle X-ray scattering and X-ray absorption spectroscopy. The catalysts are found to be sintering resistant at elevated temperatures as well as during reduction and hydrogenation reactions. In contrast to Pt particles of approximately 7 nm diameter, smaller particles of 1.8 nm in size are found to dynamically adapt their shape and oxidation state to the changes in the reaction environment. These smaller Pt particles also showed an initial deactivation in ethene hydrogenation, which is paralleled by the change in the particle shape. The subtle temperature-dependent X-ray absorbance of the 1.8 nm sized Pt particles indicates that subtle variations in the electronic structure induced by the state of reduction by electron tunnelling over the Schottky barrier between the Pt particles and the GaN support can be monitored.
机译:这篇专题文章介绍了GaN负载的Pt催化剂在乙烯加氢中的制备,表征和催化反应活性,强调了通过将程序升温反应与原位放牧相结合,在样品处理和催化过程中对材料性能进行原位表征入射小角X射线散射和X射线吸收光谱。发现该催化剂在高温下以及在还原和氢化反应期间是抗烧结的。与直径约7 nm的Pt颗粒相反,发现尺寸为1.8 nm的较小颗粒可以动态改变其形状和氧化态以适应反应环境的变化。这些较小的Pt颗粒还显示出乙烯氢化反应的初始失活,这与颗粒形状的变化平行。 1.8 nm大小的Pt颗粒的微弱的温度依赖性X射线吸收率表明,可以监测由于Pt颗粒与GaN载体之间的肖特基势垒上的电子隧穿引起的还原状态所引起的电子结构的微妙变化。

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