What is it about?
It is a result of more than 2 years struggle to convince referees that the most of the community is wrong. The article shows experimentally that in low temperature (150C) CO oxidation on Au/CeO2 there is no oxygen exchange with ceria. It was already suggested by older isotope exchange experiments bu still the ceria lattice parameter changes and Raman spectroscopy 460 cm−1 peak shift is often wrongly interpreted. This shows that the reaction mechanism is certainly not that of Mars van Krevelen - as claimed by most of the papers. The article also shows strength of in situ powder diffraction commonly treated as bulk method.
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Why is it important?
The ceria lattice parameter changes and Raman spectroscopy 460 cm−1 peak shift is related to population of Ce(3+) ions. The point is that on chemisorption on CeO2 surface, some ceria electrons are involved forming surface double layer and reversibly resulting in turning of some subsurface Ce(4+) into Ce(3+). This however has nothing to do with oxygen mobility. This stresses role of Ce(3+) in catalysis rather than oxygen mobility. Important is critical approach to the published papers and nor rewriting claims without understanding mechanisms.
Perspectives
Mainstream catalytic journals accept manuscripts only with standard methodology. Novel interdisciplinary approaches are treated with reservation and it is hard to find expert referees. This is why most of high ranked papers offer new excellent catalysts (of not repeatable preparation) analyzed by standard methods, but is not much interested in understanding of atomistic mechanism.
Professor ZBIGNIEW Antoni KASZKUR
Institute of Physical Chemistry PAS
Read the Original
This page is a summary of: In situ diffraction monitoring of nanocrystals structure evolving during catalytic reaction at their surface, Scientific Reports, January 2023, Springer Science + Business Media,
DOI: 10.1038/s41598-023-28557-5.
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