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Nat Chem. 2011 Jun 12;3(7):546-50. doi: 10.1038/nchem.1069.

Design principles for oxygen-reduction activity on perovskite oxide catalysts for fuel cells and metal-air batteries.

Author information

1
Materials Science and Engineering Department and Electrochemical Energy Laboratory, Massachusetts Institute of Technology, 31-056, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA.

Erratum in

  • Nat Chem. 2011;3(8):647.

Abstract

The prohibitive cost and scarcity of the noble-metal catalysts needed for catalysing the oxygen reduction reaction (ORR) in fuel cells and metal-air batteries limit the commercialization of these clean-energy technologies. Identifying a catalyst design principle that links material properties to the catalytic activity can accelerate the search for highly active and abundant transition-metal-oxide catalysts to replace platinum. Here, we demonstrate that the ORR activity for oxide catalysts primarily correlates to σ-orbital (e(g)) occupation and the extent of B-site transition-metal-oxygen covalency, which serves as a secondary activity descriptor. Our findings reflect the critical influences of the σ orbital and metal-oxygen covalency on the competition between O(2)(2-)/OH(-) displacement and OH(-) regeneration on surface transition-metal ions as the rate-limiting steps of the ORR, and thus highlight the importance of electronic structure in controlling oxide catalytic activity.

PMID:
21697876
DOI:
10.1038/nchem.1069

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