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平面微结构模型催化剂上方产物气体的演化——扫描质谱、蒙特卡罗和计算流体动力学的联合研究。

Product gas evolution above planar microstructured model catalysts--a combined scanning mass spectrometry, Monte Carlo, and Computational Fluid Dynamics study.

机构信息

Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm, Germany.

出版信息

J Chem Phys. 2010 Sep 7;133(9):094504. doi: 10.1063/1.3475518.

Abstract

The transport and distribution of reaction products above catalytically active Pt microstructures was studied by spatially resolved scanning mass spectrometry (SMS) in combination with Monte Carlo simulation and fluid dynamics calculations, using the oxidation of CO as test reaction. The spatial gas distribution above the Pt fields was measured via a thin quartz capillary connected to a mass spectrometer. Measurements were performed in two different pressure regimes, being characteristic for ballistic mass transfer and diffusion involving multiple collisions for the motion of CO(2) product molecules between the sample and the capillary tip, and using differently sized and shaped Pt microstructures. The tip height dependent lateral resolution of the SMS measurements as well as contributions from shadowing effects, due to the mass transport limitations between capillary tip and sample surface at close separations, were evaluated and analyzed. The data allow to define measurement and reaction conditions where effects induced by the capillary tip can be neglected ("minimal invasive measurements") and provide a basis for the evaluation of catalyst activities on microstructured model systems, e.g., for catalyst screening or studies of transport effects.

摘要

通过空间分辨扫描质谱 (SMS) 结合蒙特卡罗模拟和流体动力学计算,研究了催化活性 Pt 微结构上方反应产物的传输和分布,使用 CO 的氧化作为测试反应。通过连接到质谱仪的薄石英毛细管测量 Pt 场上方的空间气体分布。在两种不同的压力范围内进行了测量,这两种压力范围分别与弹道质量传递和扩散有关,对于 CO(2)产物分子在样品和毛细管尖端之间的运动,涉及多次碰撞,并且使用了不同大小和形状的 Pt 微结构。评估和分析了 SMS 测量的尖端高度相关的横向分辨率以及由于在接近分离时毛细管尖端和样品表面之间的质量传输限制而产生的阴影效应的贡献。这些数据可用于定义可忽略毛细管尖端引起的影响的测量和反应条件(“微创测量”),并为在微结构模型系统上评估催化剂活性提供基础,例如用于催化剂筛选或传输效应研究。

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