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用于催化活性微结构定量反应研究的扫描质谱仪。

Scanning mass spectrometer for quantitative reaction studies on catalytically active microstructures.

作者信息

Roos M, Kielbassa S, Schirling C, Häring T, Bansmann J, Behm R J

机构信息

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

出版信息

Rev Sci Instrum. 2007 Aug;78(8):084104. doi: 10.1063/1.2777167.

Abstract

We describe an apparatus for spatially resolving scanning mass spectrometry which is able to measure the gas composition above catalytically active microstructures or arrays of these microstructures with a lateral resolution of better than 100 mum under reaction conditions and which allows us to quantitatively determine reaction rates on individual microstructures. Measurements of the three-dimensional gas composition at different vertical distances and separations between active structures allow the evaluation of gas phase mass transport effects. The system is based on a piezoelectrically driven positioning substage for controlled lateral and vertical positioning of the sample under a rigidly mounted capillary probe connecting to a mass spectrometer. Measurements can be performed at pressures in the range of <10(-2)-10 mbars and temperatures between room temperature and 450 degrees C. The performance of the setup is demonstrated using the CO oxidation reaction on Pt microstructures on Si with sizes between 100 and 300 mum and distances in the same order of magnitude, evaluating CO(2) formation and CO consumption above the microstructures. The rapidly decaying lateral resolution with increasing distance between sample and probe underlines the effects of (lateral) gas transport in the room between sample and probe. The reaction rates and apparent activation energy obtained from such measurements agree with previous data on extended surfaces, demonstrating the feasibility of determining absolute reaction rates on individual microstructures.

摘要

我们描述了一种用于空间分辨扫描质谱分析的仪器,该仪器能够在反应条件下测量催化活性微结构或这些微结构阵列上方的气体成分,其横向分辨率优于100μm,并能让我们定量测定单个微结构上的反应速率。在活性结构之间不同垂直距离和间距处测量三维气体成分,有助于评估气相质量传输效应。该系统基于一个压电驱动的定位子台,用于在连接到质谱仪的刚性安装的毛细管探头下方对样品进行可控的横向和垂直定位。测量可在压力范围为<10(-2)-10毫巴以及室温至450℃的温度下进行。使用尺寸在100至300μm之间且间距在相同数量级的硅上的铂微结构上的CO氧化反应来展示该装置的性能,评估微结构上方的CO(2)形成和CO消耗。随着样品与探头之间距离增加,横向分辨率迅速衰减,这突出了样品与探头之间空间中(横向)气体传输的影响。从这些测量中获得的反应速率和表观活化能与先前关于扩展表面的数据一致,证明了测定单个微结构上绝对反应速率的可行性。

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