Electrodes
in solid-state energy devices are subjected to a variety
of thermal treatments, from film processing to device operation at
high temperatures. All these treatments influence the chemical activity
and stability of the films, as the thermally induced chemical restructuring
shapes the microstructure and the morphology. Here, we investigate
the correlation between the oxygen reduction reaction (ORR) activity
and thermal history in complex transition metal oxides, in particular,
La
0.6
Sr
0.4
CoO
3−δ
(LSC64)
thin films deposited by pulsed laser deposition. To this end, three
∼200 nm thick LSC64 films with different processing and thermal
histories were studied. A variety of surface-sensitive elemental characterization
techniques (
i.e
., low-energy ion scattering, X-ray
photoelectron spectroscopy, and secondary ion mass spectrometry) were
employed to thoroughly investigate the cationic distribution from
the outermost surface to the film/substrate interface. Moreover, electrochemical
impedance spectroscopy was used to study the activity and the stability
of the films. Our investigations revealed that, despite the initial
comparable ORR activity at 600 °C, the degradation rates of the
films differed by twofold in the long-term stability tests at 500
°C. Here, we emphasize the importance of processing and thermal
history in the elemental surface distribution, especially for the
stability of LSC64 electrodes and propose that they should be considered
as among the main pillars in the design of active surfaces.