Ambient pressure operando catalytic characterization by combining PM-IRRAS with planar laser-induced fluorescence and surface optical reflectance imaging

被引:5
作者
Ramisch, Lisa [1 ]
Pfaff, Sebastian [1 ]
Gericke, Sabrina M. [1 ]
Lundgren, Edvin [2 ]
Zetterberg, Johan [1 ]
机构
[1] Lund Univ, Combust Phys, Solvegatan 14, S-22363 Lund, Sweden
[2] Lund Univ, Div Synchrotron Radiat Res, Solvegatan 14, S-22363 Lund, Sweden
基金
瑞典研究理事会;
关键词
PM-IRRAS; Surface spectroscopy; Gas phase imaging; Reflectance microscopy; Reactor development; Operando catalysis; Mass spectrometry; CO OXIDATION; SPECTROSCOPY; ADSORPTION; PALLADIUM; PD(100); METAL;
D O I
10.1016/j.cattod.2023.114441
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
We present a combination of optical operando techniques that allow us to bridge the pressure gap in heterogeneous catalysis. By combining Polarization Modulated - InfraRed Reflection Absorption Spectroscopy (PMIRRAS) with two dimensional-Surface Optical Reflectance (2D-SOR) and Planar Laser Induced Fluorescence (PLIF), we can simultaneously measure the adsorbed species on the catalyst surface, monitor the surface oxide formation across the catalyst surface and image the gas phase right above the catalyst surface, respectively. In a single measurement, we are able to follow heterogeneous catalytic reactions temporally- and spatially resolved with all three optical techniques, which are additionally supported by Mass Spectrometry (MS). To validate the experimental setup, we perform two experiments studying CO oxidation on Pd(100) at 150 mbar and 910 mbar by ramping the sample temperature. PM-IRRAS and 2D-SOR reveal that the formation of well-defined ultrathin surface oxide coincides with the disappearance of CO adsorption on the surface. At the same time, PLIF and MS confirm the simultaneous transition into a mass-transfer-limited (MTL) regime. A difference between 150 and 910 mbar can be seen in the light-off temperature caused by different partial pressures of CO and in the spatial distribution of the gas cloud across the surface in space caused by gas diffusion. This emphasizes the need for spatially-resolved gas phase diagnostics in heterogeneous catalysis. The combination of all techniques aids our understanding of the gas-surface interaction.
引用
收藏
页数:10
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