Equilibrium oxygen storage capacity of ultrathin CeO2-δ depends non-monotonically on large biaxial strain
| العنوان: | Equilibrium oxygen storage capacity of ultrathin CeO2-δ depends non-monotonically on large biaxial strain |
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| المؤلفون: | Zixuan Guan, Aleksandra Vojvodic, Matteo Monti, Max García-Melchor, Andrey Shavorskiy, William C. Chueh, Robert Sinclair, Yezhou Shi, Hendrik Bluhm, Chirranjeevi Balaji Gopal, Sang Chul Lee |
| المصدر: | Nature communications, vol 8, iss 1 Nature Communications, Vol 8, Iss 1, Pp 1-12 (2017) |
| بيانات النشر: | Springer Science and Business Media LLC, 2017. |
| سنة النشر: | 2017 |
| مصطلحات موضوعية: | Solid-state chemistry, Multidisciplinary, Materials science, Tension (physics), Science, Oxide, General Physics and Astronomy, Nanotechnology, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Compression (physics), 01 natural sciences, General Biochemistry, Genetics and Molecular Biology, 0104 chemical sciences, Tetragonal crystal system, chemistry.chemical_compound, X-ray photoelectron spectroscopy, chemistry, Chemical physics, Ab initio quantum chemistry methods, 0210 nano-technology, Ambient pressure |
| الوصف: | Elastic strain is being increasingly employed to enhance the catalytic properties of mixed ion–electron conducting oxides. However, its effect on oxygen storage capacity is not well established. Here, we fabricate ultrathin, coherently strained films of CeO2-δ between 5.6% biaxial compression and 2.1% tension. In situ ambient pressure X-ray photoelectron spectroscopy reveals up to a fourfold enhancement in equilibrium oxygen storage capacity under both compression and tension. This non-monotonic variation with strain departs from the conventional wisdom based on a chemical expansion dominated behaviour. Through depth profiling, film thickness variations and a coupled photoemission–thermodynamic analysis of space-charge effects, we show that the enhanced reducibility is not dominated by interfacial effects. On the basis of ab initio calculations of oxygen vacancy formation incorporating defect interactions and vibrational contributions, we suggest that the non-monotonicity arises from the tetragonal distortion under large biaxial strain. These results may guide the rational engineering of multilayer and core–shell oxide nanomaterials. |
| وصف الملف: | application/pdf |
| تدمد: | 2041-1723 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::4ef4b4f5bd788dc7a337c86bf2f25b8a https://doi.org/10.1038/ncomms15360 |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....4ef4b4f5bd788dc7a337c86bf2f25b8a |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 20411723 |
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