| Autor: |
VeneziaThese authors contributed equally., B., Cao, E., Matam, S. K., Waldron, C., Cibin, G., Gibson, E. K., Golunski, S., Wells, P. P., Silverwood, I., Catlow, C. R. A., Sankar, G., Gavriilidis, A. |
| Zdroj: |
Catalysis Science & Technology; 2020, Vol. 10 Issue: 23 p7842-7856, 15p |
| Abstrakt: |
OperandoX-ray absorption spectroscopy (XAS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and mass spectrometry (MS) provide complementary information on the catalyst structure, surface reaction mechanisms and activity relationships. The powerful combination of the techniques has been the driving force to design and engineer suitable spectroscopic operandoreactors that can mitigate limitations inherent to conventional reaction cells and facilitate experiments under kinetic regimes. Microreactors have recently emerged as effective spectroscopic operandocells due to their plug-flow type operation with no dead volume and negligible mass and heat transfer resistances. Here we present a novel microfabricated reactor that can be used for both operandoXAS and DRIFTS studies. The reactor has a glass–silicon–glass sandwich-like structure with a reaction channel (3000 μm × 600 μm; width × depth) packed with a catalyst bed (ca.25 mg) and placed sideways to the X-ray beam, while the infrared beam illuminates the catalyst bed from the top. The outlet of the reactor is connected to MS for continuous monitoring of the reactor effluent. The feasibility of the microreactor is demonstrated by conducting two reactions: i) combustion of methane over 2 wt% Pd/Al2O3studied by operandoXAS at the Pd K-edge and ii) CO oxidation over 1 wt% Pt/Al2O3catalyst studied by operandoDRIFTS. The former shows that palladium is in an oxidised state at all studied temperatures, 250, 300, 350, 400 °C and the latter shows the presence of linearly adsorbed CO on the platinum surface. Furthermore, temperature-resolved reduction of palladium catalyst with methane and CO oxidation over platinum catalyst are also studied. Based on these results, the catalyst structure and surface reaction dynamics are discussed, which demonstrate not only the applicability and versatility of the microreactor for combined operandoXAS and DRIFTS studies, but also illustrate the unique advantages of the microreactor for high space velocity and transient response experiments. |
| Databáze: |
Supplemental Index |
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