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Elucidating Oxygen Reduction Active Sites in Pyrolyzed Metal–Nitrogen Coordinated Non-Precious-Metal Electrocatalyst Systems
Open accessAbstract
Abstract Detailed understanding of the nature of the active centers in non-precious-metal-based electrocatalyst, and their role in oxygen reduction reaction (ORR) mechanistic pathways will have a profound effect on successful commercialization of emission-free energy devices such as fuel cells. Recently, using pyrolyzed model structures of iron porphyrins, we have demonstrated that a covalent integration of the Fe–Nx sites into π-conjugated carbon basal plane modifies electron donating/withdrawing capability of the carbonaceous ligand, consequently improving ORR activity. Here, we employ a combination of in situ X-ray spectroscopy and electrochemical methods to identify the various structural and functional forms of the active centers in non-heme Fe/N/C catalysts. Both methods corroboratively confirm the single site 2e– × 2e– mechanism in alkaline media on the primary Fe2+–N4 centers and the dual-site 2e– × 2e– mechanism in acid media with the significant role of the surface bound coexisting Fe/FexOy nanoparticles (NPs) as the secondary active sites.
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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
Cited by
Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction
Kulkarni, A., Siahrostami, S., Patel, A., & Nørskov, J. K. (2018) · Chemical Reviews · doi:10.1021/acs.chemrev.7b00488 · Cited by 2,742
Jiang, W.-J., Gu, L., Li, L., Zhang, Y., Zhang, X., Zhang, L.-J., Wang, J.-Q., Hu, J.-S., Wei, Z., & Wan, L.-J. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b00757 · Cited by 1,765
Sa, Y. J., Seo, D.-J., Woo, J., Lim, J. T., Cheon, J. Y., Yang, S. Y., Lee, J. M., Kang, D., Shin, T. J., Shin, H. S., et al. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b09470 · Cited by 746
Wu, G., Santandreu, A., Kellogg, W., Gupta, S., Ogoke, O., Zhang, H., Wang, H.-L., & Dai, L. (2016) · Nano Energy · doi:10.1016/j.nanoen.2015.12.032 · Cited by 744
Mun, Y., Lee, S., Kim, K., Kim, S., Lee, S., Han, J. W., & Lee, J. (2019) · Journal of the American Chemical Society · doi:10.1021/jacs.8b13543 · Cited by 710
Metadata
- Authors
- Tylus, U., Jia, Q., Strickland, K., Ramaswamy, N., Serov, A., Atanassov, P., & Mukerjee, S.
- Venue
- The Journal of Physical Chemistry C
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-04-17
- Volume
- 118
- Issue
- 17
- Pages
- 8999-9008
- ISSN
- 1932-7447 (ISSN-L)
- 1932-7455
- OpenAlex
- W2329760721
- Cited by
- 541
- References
- 2
- FWCI
- 19.43
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Tylus, U., Jia, Q., Strickland, K., Ramaswamy, N., Serov, A., Atanassov, P., & Mukerjee, S. (2014). Elucidating Oxygen Reduction Active Sites in Pyrolyzed Metal–Nitrogen Coordinated Non-Precious-Metal Electrocatalyst Systems. The Journal of Physical Chemistry C. https://doi.org/10.1021/jp500781v
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