Material Discovery and Design Principles for Stable, High Activity Perovskite Cathodes for Solid Oxide Fuel Cells

Abstract

Critical to the development of improved solid oxide fuel cell (SOFC) technology are novel compounds with high oxygen reduction reaction (ORR) catalytic activity and robust stability under cathode operating conditions. Approximately 2145 distinct perovskite compositions are screened for potential use as high activity, stable SOFC cathodes, and it is verified that the screening methodology qualitatively reproduces the experimental activity, stability, and conduction properties of well-studied cathode materials. The calculated oxygen p-band center is used as a first principle-based descriptor of the surface exchange coefficient (k*), which in turn correlates with cathode ORR activity. Convex hull analysis is used under operating conditions in the presence of oxygen, hydrogen, and water vapor to determine thermodynamic stability. This search has yielded 52 potential cathode materials with good predicted stability in typical SOFC operating conditions and predicted k* on par with leading ORR perovskite catalysts. The established trends in predicted k* and stability are used to suggest methods of improving the performance of known promising compounds. The material design strategies and new materials discovered in the computational search help enable the development of high activity, stable compounds for use in future solid oxide fuel cells and related applications.

References in corpus (7)

• Achieving fast oxygen diffusion in perovskites by cation ordering
• High-Throughput Computational Screening of thermal conductivity, Debye temperature and Grüneisen parameter using a quasi-harmonic Debye Model
• The elastic constants of MgSiO3 perovskite at pressures and temperatures of the Earth's mantle
• Understanding and controlling the work function of perovskite oxides using Density Functional Theory
• Factors controlling oxygen migration barriers in perovskites
• Oxygen Point Defect Chemistry in Ruddlesden-Popper Oxides (La${}_{1-x}$Sr${}_x$)${}_2$MO${}_{4\pm \delta }$ (M = Co, Ni, Cu)
• The MAterials Simulation Toolkit (MAST) for atomistic modeling of defects and diffusion

Cited by in corpus (7)

• Predicting the thermodynamic stability of perovskite oxides using machine learning models
• Assessing correlations of perovskite catalytic performance with electronic structure descriptors
• The role of decomposition reactions in assessing first-principles predictions of solid stability
• Materials Discovery of Stable and Nontoxic Halide Perovskite Materials for High-Efficiency Solar Cells
• Analogical discovery of disordered perovskite oxides by crystal structure information hidden in unsupervised material fingerprints
• Solid phase epitaxial growth of the correlated-electron transparent conducting oxide SrVO3
• Discovery and Engineering of Low Work Function Perovskite Materials