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用于催化研究的新型类反应器高温近常压扫描隧道显微镜的设计

Design of a new reactor-like high temperature near ambient pressure scanning tunneling microscope for catalysis studies.

作者信息

Tao Franklin Feng, Nguyen Luan, Zhang Shiran

机构信息

Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, USA.

出版信息

Rev Sci Instrum. 2013 Mar;84(3):034101. doi: 10.1063/1.4792673.

DOI:10.1063/1.4792673
PMID:23556828
Abstract

Here, we present the design of a new reactor-like high-temperature near ambient pressure scanning tunneling microscope (HT-NAP-STM) for catalysis studies. This HT-NAP-STM was designed for exploration of structures of catalyst surfaces at atomic scale during catalysis or under reaction conditions. In this HT-NAP-STM, the minimized reactor with a volume of reactant gases of ∼10 ml is thermally isolated from the STM room through a shielding dome installed between the reactor and STM room. An aperture on the dome was made to allow tip to approach to or retract from a catalyst surface in the reactor. This dome minimizes thermal diffusion from hot gas of the reactor to the STM room and thus remains STM head at a constant temperature near to room temperature, allowing observation of surface structures at atomic scale under reaction conditions or during catalysis with minimized thermal drift. The integrated quadrupole mass spectrometer can simultaneously measure products during visualization of surface structure of a catalyst. This synergy allows building an intrinsic correlation between surface structure and its catalytic performance. This correlation offers important insights for understanding of catalysis. Tests were done on graphite in ambient environment, Pt(111) in CO, graphene on Ru(0001) in UHV at high temperature and gaseous environment at high temperature. Atom-resolved surface structure of graphene on Ru(0001) at 500 K in a gaseous environment of 25 Torr was identified.

摘要

在此,我们展示了一种用于催化研究的新型类似反应器的高温近常压扫描隧道显微镜(HT-NAP-STM)的设计。这种HT-NAP-STM旨在探索催化过程中或反应条件下催化剂表面的原子尺度结构。在这种HT-NAP-STM中,体积约为10毫升反应气体的最小化反应器通过安装在反应器和STM室之间的屏蔽穹顶与STM室热隔离。穹顶上开有一个孔,以便探针能接近或从反应器中的催化剂表面缩回。这个穹顶使反应器热气体向STM室的热扩散最小化,从而使STM探头保持在接近室温的恒定温度,允许在反应条件下或催化过程中以最小的热漂移观察原子尺度的表面结构。集成的四极杆质谱仪可以在观察催化剂表面结构的同时测量产物。这种协同作用使得能够建立表面结构与其催化性能之间的内在关联。这种关联为理解催化作用提供了重要的见解。在环境气氛下对石墨、在CO气氛中对Pt(111)、在超高真空高温下以及在高温气态环境下对Ru(0001)上的石墨烯进行了测试。在25托的气态环境中,在500 K温度下确定了Ru(0001)上石墨烯的原子分辨表面结构。

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引用本文的文献

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Heterogeneous catalysis: More than skimming the surface.多相催化:不止于表面掠过。
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