Mechanism for enhanced oxygen reduction kinetics at the (La,Sr)CoO3–δ/(La,Sr)2CoO4+δ hetero-interface

Han, Jeong Woo; Yildiz, Bilge

doi:10.1039/c2ee03592h

Mechanism for enhanced oxygen reduction kinetics at the (La,Sr)CoO_3–δ/(La,Sr)₂CoO_4+δ hetero-interface

Journal Article · Wed May 30 00:00:00 EDT 2012 · Energy & Environmental Science

DOI:https://doi.org/10.1039/c2ee03592h· OSTI ID:1557717

Han, Jeong Woo ^[1]; Yildiz, Bilge ^[2]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Office of Scientific and Technical Information (OSTI)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

The recently reported fast oxygen reduction kinetics at the interface of (La,Sr)CoO_3–δ (LSC₁₁₃) and (La,Sr)₂CoO_4+δ(LSC₂₁₄) phases opened up new questions for the potential role of dissimilar interfaces in advanced cathodes for solid oxide fuel cells (SOFCs). Using first-principles based calculations in the framework of density functional theory, we quantitatively probed the possible mechanisms that govern the oxygen reduction activity enhancement at this hetero-interface as a model system. Our findings show that both the strongly anisotropic oxygen incorporation kinetics on the LSC₂₁₄ and the lattice strain in the vicinity of the interface are important contributors to such enhancement. The LSC₂₁₄(100) surface exposed to the ambient at the LSC₁₁₃/LSC₂₁₄ interface facilitates oxygen incorporation because the oxygen molecules very favorably adsorb onto it compared to the LSC₂₁₄(001) and LSC₁₁₃(001) surfaces, providing a large source term for oxygen incorporation. Lattice strain field present near the hetero-interface accelerates oxygen incorporation kinetics especially on the LSC₁₁₃(001) surface. At 500 °C, 4 × 10² times faster oxygen incorporation kinetics are predicted in the vicinity of the LSC₁₁₃/LSC₂₁₄ hetero-interface with 50% Sr-doped LSC₂₁₄ compared to that on the single phase LSC₁₁₃(001) surface. Contributions from both the anisotropy and the local strain effects are of comparable magnitude. Furthermore, the insights obtained in this work suggest that hetero-structures, which have a large area of (100) surfaces and smaller thickness in the [001] direction of the Ruddlesden–Popper phases, and larger tensile strain near the interface would be promising for high-performance cathodes.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0002633

OSTI ID:: 1557717

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 9 Vol. 5; ISSN EESNBY; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

(La
Sr)2CoO4+δ
(La
Sr)CoO3
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Ruddlesden-Popper
anisotropy
cathode
density functional theory
oxygen reduction reaction
perovskite
solid oxide fuel cell
strain