Journal
TOPICS IN CATALYSIS
Volume 52, Issue 10, Pages 1410-1424Publisher
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-009-9321-2
Keywords
Synchronous DRIFTS/EXAFS; Quick and energy dispersive EXAFS; Time resolved; CO NO reaction
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Examples of the application of a synchronous DRIFTS/EXAFS/mass spectrometry (MS) methodology to the study of dilute (a parts per thousand currency sign 1wt%) Rh/Al2O3 catalysts are discussed. These are used to explore the potential of this approach for understanding of the behaviour of supported metal catalysts in a single shot, and in the often preferred regime of low (< 1 wt%) loadings of active precious metals. Firstly, the sequential interaction of NO (323 K) and then CO (373 K) with reduced, 0.5 wt% Rh/Al2O3 catalysts is studied. Infrared spectroscopy indicates that two surface species (a bent Rh(NO-) and Rh(CO)(2) species) can be created using this sequential gas absorption/reaction method with minimal interference from other carbonyl or nitrosyl species. As such the potential for a reliable structural characterisation of the local structure of these species by EXAFS becomes possible. However, in contrast to the infrared spectroscopy, analysis of the EXAFS data also indicates that, even for such low loaded Rh systems, oxidative disruption of the Rh by the NO and CO is not complete and that bonding typical of small Rh clusters persists in both cases. The possible sources of this apparent spectroscopic difference of opinion are discussed. Secondly, 1wt% Rh/Al2O3 catalysts are studied using dispersive EXAFS at 573 K with 100 ms time resolution, during a redox switching event involving a reducing feedstock comprising just 3000 ppm of CO and 3000 ppm of NO. It is shown that highly useful and insightful time resolved and synchronously obtained XANES/EXAFS/IR data can be obtained even in this dilute Rh and more realistic case. Additional data, regarding the overall performance of the experiment, as currently implemented at the ESRF, along with a discussion of where enhanced performance might be yet still be gained, are also given.
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