Oxygen Reduction Activity on Perovskite Oxide Surfaces: A Comparative First-Principles Study of LaMnO3, LaFeO3, and LaCrO3

• Published in: Journal of physical chemistry. C Vol. 117; no. 5; pp. 2106 - 2112
• Main Authors: Wang, Yan, Cheng, Hai-Ping
• Format: Journal Article
• Language: English
• Published: Columbus, OH American Chemical Society 07-02-2013
• Subjects: Chemistry; Electrochemistry; Exact sciences and technology; General and physical chemistry; Miscellaneous (electroosmosis, electrophoresis, electrochromism, electrocrystallization, ...); Chemical reduction; Hartree-Fock calculations; Oxygen; Perovskite type compound; Lanthanum Chromites; Density functional method; Generalized gradient approximation; Lanthanum Manganites
• ISSN: 1932-7447; 1932-7455
• DOI: 10.1021/jp309203k

The understanding of oxygen reduction reaction (ORR) activity on perovskite oxide surfaces is essential for promising future fuel cell applications. We report a comparative study of the ORR mechanisms on LaBO3 (B = Mn, Fe, Cr) surfaces by first-principles calculations based on density functional theory (DFT). Results obtained from varied DFT methods such as generalized gradient approximation (GGA), GGA+U and the hybrid Hartree–Fock density functional method are reported for comparative purposes. We find that the results calculated from hybrid-functional method suggest that the order of ORR activity is LaMnO3 > LaCrO3 > LaFeO3, which is in better agreement with recent experimental results (Suntivich et al., Nature Chemistry 2011, 3, 546) than those using the GGA or GGA+U method.