Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 51, Pages 16399-16404Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201709199
Keywords
CeO2; dioxygen activation; IRRAS; surface chemistry; vibrational spectroscopy
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Funding
- Helmholtz association through the Science and Technology of Nanosystems Program [432202]
- China Scholarship Council (CSC)
- Helmholtz Research School Energy-related catalysis
- Fonds der Chemischen Industrie (FCI)
- UniCat Cluster of Excellence
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An atomic-level understanding of dioxygen activation on metal oxides remains one of the major challenges in heterogeneous catalysis. By performing a thorough surface-science study of all three low-index single-crystal surfaces of ceria, probably the most important redox catalysts, we provide a direct spectroscopic characterization of reactive dioxygen species at defect sites on the reduced ceria (110) and (100) surfaces. Surprisingly, neither of these superoxo and peroxo species was found on ceria (111), the thermodynamically most stable surface of this oxide. Applying density functional theory, we could relate these apparently inconsistent findings to a subsurface diffusion ofO vacancies on (111) substrates, but not on the less-closely packed surfaces. These observations resolve a long standing debate concerning the location of O vacancies on ceria surfaces and the activation of O-2 on ceria powders.
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