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One Beam, Dual Insights: Simultaneous Chemical and Structural Changes in Nanopatterned Ceria under Reaction
Adva Ben Yaacov1, Maximilian Jaugstetter2, Heath Kersell3
1Department of Chemical and Biological Physics, Weizmann Institute of Science, 234 Herzl Street, 76100 Rehovot, Israel.
None:
Ceria's interaction with hydrogen can proceed through multiple chemical forms (hydride, hydroxyl, and oxyhydroxide-like), with consequences for the oxidation state, density, and morphology that are rarely tracked in the same evolving state. Here we show that under mild H2 (and H2 and CO2) environments nanopatterned ceria undergoes oxidation-state changes accompanied by hydrogen incorporation that increases the effective electron density, establishing the following order: CeO2Hy > CeO2 > CeO2-xHy > CeO2-x. In parallel, the surface roughens in a chemically specific manner, with the largest changes coinciding with conditions where incorporated hydrogen is driven to react with oxygen supplied either by air exposure between experiments or by added CO2. We obtained these insights by using a single X-ray beam to simultaneously perform ambient-pressure X-ray photoelectron spectroscopy and grazing-incidence X-ray scattering on the same sample spot. Single-mode measurements can miss key ceria-H2 transformations relevant to optimizing ceria-based hydrogenation catalysts and supports.
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