Equilibrium oxygen storage capacity of ultrathin CeO2-δ depends non-monotonically on large biaxial strain

Chirranjeevi Balaji Gopal, Max García-Melchor, Sang Chul Lee, Yezhou Shi, Andrey Shavorskiy, Matteo Monti, Zixuan Guan, Robert Sinclair, Hendrik Bluhm, Aleksandra Vojvodic () and William C. Chueh ()
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Chirranjeevi Balaji Gopal: Stanford University
Max García-Melchor: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Sang Chul Lee: Stanford University
Yezhou Shi: Stanford University
Andrey Shavorskiy: MAX IV Laboratory, Lund University
Matteo Monti: Stanford University
Zixuan Guan: Stanford University
Robert Sinclair: Stanford University
Hendrik Bluhm: Lawrence Berkeley National Laboratory
Aleksandra Vojvodic: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
William C. Chueh: Stanford University

Nature Communications, 2017, vol. 8, issue 1, 1-12

Abstract: Abstract 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.

Date: 2017
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DOI: 10.1038/ncomms15360

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