Pfaff Sebastian, Larsson Alfred, Orlov Dmytro, Rämisch Lisa, Gericke Sabrina M, Lundgren Edvin, Zetterberg Johan
Combustion Research Facility, Sandia National Laboratories, 7011 East Ave, Livermore, California 94550, United States.
Division of Synchrotron Radiation Research, Lund University, Sölvegatan 14, S-22363 Lund, Sweden.
ACS Appl Mater Interfaces. 2024 Jan 10;16(1):444-453. doi: 10.1021/acsami.3c11341. Epub 2023 Dec 18.
Industrial catalysts are complex materials systems operating in harsh environments. The active parts of the catalysts are nanoparticles that expose different facets with different surface orientations at which the catalytic reactions occur. However, these facets are close to impossible to study in detail under industrially relevant operating conditions. Instead, simpler model systems, such as single crystals with a well-defined surface orientation, have been successfully used to study gas-surface interactions such as adsorption and desorption, surface oxidation, and oxidation/reduction reactions. To more closely mimic the many facets exhibited by nanoparticles and thereby close the so-called materials gap, there has also been a recent move toward using polycrystalline surfaces and curved crystals. However, these studies are limited either by the pressure or spatial resolution at realistic pressures or by the number of surfaces studied simultaneously. In this work, we demonstrate the use of reflectance microscopy to study a vast number of catalytically active surfaces simultaneously under realistic and identical reaction conditions. As a proof of concept, we have conducted an experiment to study CO oxidation over a Pd polycrystal, where the polycrystalline surface acts as a collection of many single-crystal surfaces. Finally, we visualized the resulting data by plotting the reflectivity as a function of surface orientation. We think the techniques and visualization methods introduced in this work will be key toward bridging the materials gap in catalysis.
工业催化剂是在恶劣环境中运行的复杂材料体系。催化剂的活性部分是纳米颗粒,这些纳米颗粒暴露出具有不同表面取向的不同晶面,催化反应就在这些晶面上发生。然而,在工业相关的操作条件下,几乎不可能详细研究这些晶面。相反,更简单的模型体系,如具有明确表面取向的单晶,已成功用于研究气-固表面相互作用,如吸附和解吸、表面氧化以及氧化/还原反应。为了更紧密地模拟纳米颗粒所呈现的众多晶面,从而缩小所谓的材料差距,最近也有人转向使用多晶表面和弯曲晶体。然而,这些研究要么受到实际压力下的压力或空间分辨率的限制,要么受到同时研究的表面数量的限制。在这项工作中,我们展示了使用反射显微镜在实际且相同的反应条件下同时研究大量催化活性表面。作为概念验证,我们进行了一项实验,研究钯多晶上的一氧化碳氧化反应,其中多晶表面充当许多单晶表面的集合。最后,我们通过绘制反射率作为表面取向的函数来直观呈现所得数据。我们认为这项工作中引入的技术和可视化方法将是弥合催化领域材料差距的关键。