Identifying
the Origin of the Limiting Process in
a Double Perovskite PrBa0.5Sr0.5Co1.5Fe0.5O5+δ Thin-Film Electrode for Solid
Oxide Fuel Cells
Posted on 2019-07-01 - 18:33
Oxygen
reduction reaction in a double perovskite material, PrBa0.5Sr0.5Co1.5Fe0.5O5+δ (PBSCF), was studied for application as a cathode in a solid oxide
fuel cell (SOFC). Electrochemical measurements were performed on a
geometrically well-defined dense thin-film (0.8–2 μm
thickness) electrode, fabricated as a symmetric cell. In combination
with density functional theory (DFT) and molecular dynamics (MD) simulations,
experiments provided an insight into the operating mechanism of the
SOFC material tested at an open-circuit voltage. The dense thin-film
electrode of PBSCF showed a thickness-dependent electrochemical performance,
suggesting bulk diffusion limitation. To understand the origin of
this diffusion-limiting electrochemical performance, DFT calculations
were utilized to calculate the surface (γ) and oxygen vacancy
formation (EOV) energies. For example, EOV in the Pr plane (190 kJ/mol) of PBSCF was
measured to be lower than that of the BaSr plane (EOV = 297 kJ/mol). In addition, oxygen vacancies were difficult
to be created in the BaSr/CoFe terminal surface (EOV = 341.6 kJ/mol) as compared to other terminal surfaces.
MD simulations further elaborated on the nature of cation disordering
in the surface and subsurface regions, consequently leading to the
preferential segregation of the Ba cations to the surface, which is
a known phenomenon in such double perovskite materials. Because of
cation disordering and segregation of Ba species, the oxygen anion
diffusivity (∼10–12 cm2 s–1), calculated from MD, in the near-surface region
was observed to be 2 orders of magnitude lesser than that of the bulk
(D = 2.98 × 10–10 cm2 s–1) of the material at 973 K. Surface characterization
of the thin-film electrode using X-ray photoelectron spectroscopy
was indicative of a nonperovskite Ba2+ phase on the electrode
surface. The segregation of Ba cations was linked with the transport
of oxygen anions, which was limiting the electrochemical performance
of the electrode.
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Anjum, Uzma; Khan, Tuhin Suvra; Agarwal, Manish; Haider, M. Ali (2019). Identifying
the Origin of the Limiting Process in
a Double Perovskite PrBa0.5Sr0.5Co1.5Fe0.5O5+δ Thin-Film Electrode for Solid
Oxide Fuel Cells. ACS Publications. Collection. https://doi.org/10.1021/acsami.9b06666