Surface chemistry and porosity engineering through etching reveal ultrafast oxygen reduction kinetics below 400 °C in B-site exposed (La,Sr)(Co,Fe)O3 thin-films

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Oxides are critical materials for energy devices like solid oxide cells, catalysts, and membranes. Their performance is often limited by their catalytic activity at reduced temperatures. In this work, a simple etching process with acetic acid at room temperature was used to investigate how oxygen exchange is influenced by surface chemistry and mesoporous structuring in single-crystalline epitaxial (La0.60Sr0.40)0.95(Co0.20Fe0.80)O3. Using low energy ion scattering and electrical measurements, it is shown that increasing the B-site transition metal cation surface exposure (most notably with Fe) leads to strongly reduced activation energy from Ea≈1 eV to Ea ≈0.4 eV for oxygen exchange and an order of magnitude increased oxygen exchange kinetics below 400 °C. Increasing the active area by ~200% via mesoporous structuring leads to increased oxygen reduction rates by the same percentage. Density functional calculations indicate that a B-site exposed surface with high oxygen vacancy concentration can explain the experimental results. The work opens a pathway to tune surfaces and optimize oxygen exchange for energy devices.

40 Engineering, 4016 Materials Engineering, 34 Chemical Sciences, 3406 Physical Chemistry, 7 Affordable and Clean Energy
Journal Title
Journal of Power Sources
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Elsevier BV
Engineering and Physical Sciences Research Council (EP/P007767/1)
Royal Academy of Engineering (RAEng) (CiET1819\24)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (101017709)
EPSRC (EP/T012218/1)
European Commission Horizon 2020 (H2020) ERC (882929)