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Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells
Open accessAbstract
Fe-based catalytic sites for the reduction of oxygen in acidic medium have been identified by (57)Fe Mössbauer spectroscopy of Fe/N/C catalysts containing 0.03 to 1.55 wt% Fe, which were prepared by impregnation of iron acetate on carbon black followed by heat-treatment in NH(3) at 950 °C. Four different Fe-species were detected at all iron concentrations: three doublets assigned to molecular FeN(4)-like sites with their ferrous ions in a low (D1), intermediate (D2) or high (D3) spin state, and two other doublets assigned to a single Fe-species (D4 and D5) consisting of surface oxidized nitride nanoparticles (Fe(x)N, with x≤ 2.1). A fifth Fe-species appears only in those catalysts with Fe-contents ≥0.27 wt%. It is characterized by a very broad singlet, which has been assigned to incomplete FeN(4)-like sites that quickly dissolve in contact with an acid. Among the five Fe-species identified in these catalysts, only D1 and D3 display catalytic activity for the oxygen reduction reaction (ORR) in the acid medium, with D3 featuring a composite structure with a protonated neighbour basic nitrogen and being by far the most active species, with an estimated turn over frequency for the ORR of 11.4 e(-) per site per s at 0.8 V vs. RHE. Moreover, all D1 sites and between 1/2 and 2/3 of the D3 sites are acid-resistant. A scheme for the mechanism of site formation upon heat-treatment is also proposed. This identification of the ORR-active sites in these catalysts is of crucial importance to design strategies to improve the catalytic activity and stability of these materials.
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Gasteiger, H. A., Kocha, S. S., Sompalli, B., & Wagner, F. T. (2005) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2004.06.021 · Cited by 4,876
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
Wu, G., More, K. L., Johnston, C. M., & Zelenay, P. (2011) · Science · doi:10.1126/science.1200832 · Cited by 3,984
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Recent advancements in Pt and Pt-free catalysts for oxygen reduction reaction
Nie, Y., Li, L., & Wei, Z. (2015) · Chemical Society Reviews · doi:10.1039/c4cs00484a · Cited by 2,156
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Liu, S., Li, C., Zachman, M. J., Zeng, Y., Yu, H., Li, B., Wang, M., Braaten, J., Liu, J., Meyer, H. M., et al. (2022) · Nature Energy · doi:10.1038/s41560-022-01062-1 · Cited by 733
High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites
Zhang, H., Chung, H. T., Cullen, D. A., Wagner, S., Kramm, U. I., More, K. L., Zelenay, P., & Wu, G. (2019) · Energy & Environmental Science · doi:10.1039/c9ee00877b · Cited by 616
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Metadata
- Authors
- Kramm, U. I., Herranz, J., Larouche, N., Arruda, T. M., Lefèvre, M., Jaouen, F., Bogdanoff, P., Fiechter, S., Abs-Wurmbach, I., Mukerjee, S., & Dodelet, J.-P.
- Venue
- Physical Chemistry Chemical Physics
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2012
- Volume
- 14
- Issue
- 33
- Pages
- 11673
- ISSN
- 1463-9076 (ISSN-L)
- 1463-9084
- OpenAlex
- W2012759651
- Cited by
- 714
- References
- 2
- FWCI
- 13.12
- Type
- journal article
- Language
- en
- Open access
- green
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- Kramm, U. I., Herranz, J., Larouche, N., Arruda, T. M., Lefèvre, M., Jaouen, F., Bogdanoff, P., Fiechter, S., Abs-Wurmbach, I., Mukerjee, S., & Dodelet, J.-P. (2012). Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells. Physical Chemistry Chemical Physics. https://doi.org/10.1039/c2cp41957b
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