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Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst

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Science  04 Aug 2017:
Vol. 357, Issue 6350, pp. 479-484
DOI: 10.1126/science.aan2255

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Replacing platinum in air-fed fuel cells

Replacing expensive and scarce platinum catalysts in polymer electrolyte membrane fuel cells for the oxygen reduction reaction (ORR) with ones based on non-noble metals would speed up the adoption of hydrogen fuel vehicles. Most of the candidate replacement catalysts that have shown high performance do so only when running on pure oxygen. Chung et al. developed an iron-nitrogen-carbon catalyst from two nitrogen precursors that forms a high-porosity structure and exhibits high ORR performance when running on air. The proposed catalytically active site is FeN4.

Science, this issue p. 479

Abstract

Platinum group metal–free (PGM-free) metal-nitrogen-carbon catalysts have emerged as a promising alternative to their costly platinum (Pt)–based counterparts in polymer electrolyte fuel cells (PEFCs) but still face some major challenges, including (i) the identification of the most relevant catalytic site for the oxygen reduction reaction (ORR) and (ii) demonstration of competitive PEFC performance under automotive-application conditions in the hydrogen (H2)–air fuel cell. Herein, we demonstrate H2-air performance gains achieved with an iron-nitrogen-carbon catalyst synthesized with two nitrogen precursors that developed hierarchical porosity. Current densities recorded in the kinetic region of cathode operation, at fuel cell voltages greater than ~0.75 V, were the same as those obtained with a Pt cathode at a loading of 0.1 milligram of Pt per centimeter squared. The proposed catalytic active site, carbon-embedded nitrogen-coordinated iron (FeN4), was directly visualized with aberration-corrected scanning transmission electron microscopy, and the contributions of these active sites associated with specific lattice-level carbon structures were explored computationally.

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