The DOI matches its Crossref record; 83 of the 83 references it cites were found in a registry or an index.
A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts
Open accessAbstract
Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum catalysts for the oxygen reduction reaction (ORR) in fuel cells; however, their active site structures remain poorly understood. A leading postulate is that the iron-containing active sites exist primarily in a pyridinic Fe-N 4 ligation environment, yet, molecular model catalysts generally feature pyrrolic coordination. Herein, we report a molecular pyridinic hexaazacyclophane macrocycle, (phen 2 N 2 )Fe, and compare its spectroscopic, electrochemical, and catalytic properties for ORR to a typical Fe-N-C material and prototypical pyrrolic iron macrocycles. N 1s XPS and XAS signatures for (phen 2 N 2 )Fe are remarkably similar to those of Fe-N-C. Electrochemical studies reveal that (phen 2 N 2 )Fe has a relatively high Fe(III/II) potential with a correlated ORR onset potential within 150 mV of Fe-N-C. Unlike the pyrrolic macrocycles, (phen 2 N 2 )Fe displays excellent selectivity for four-electron ORR, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data demonstrate that (phen 2 N 2 )Fe is a more effective model of Fe-N-C active sites relative to the pyrrolic iron macrocycles, thereby establishing a new molecular platform that can aid understanding of this important class of catalytic materials.
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Cites
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Cited by
Zhao, Y., Adiyeri Saseendran, D. P., Huang, C., Triana, C. A., Marks, W. R., Chen, H., Zhao, H., & Patzke, G. R. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00515 · Cited by 802
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Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies
Yang, Y., Peltier, C. R., Zeng, R., Schimmenti, R., Li, Q., Huang, X., Yan, Z., Potsi, G., Selhorst, R., Lu, X., et al. (2022) · Chemical Reviews · doi:10.1021/acs.chemrev.1c00331 · Cited by 544
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Single-Atom (Iron-Based) Catalysts: Synthesis and Applications
Singh, B., Gawande, M. B., Kute, A. D., Varma, R. S., Fornasiero, P., McNeice, P., Jagadeesh, R. V., Beller, M., & Zbořil, R. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.1c00158 · Cited by 373
Metadata
- Authors
- Marshall-Roth, T., Libretto, N. J., Wrobel, A. T., Anderton, K. J., Pegis, M. L., Ricke, N. D., Voorhis, T. V., Miller, J. T., & Surendranath, Y.
- Venue
- Nature Communications
- Published
- 2020-10-19
- Volume
- 11
- Issue
- 1
- Pages
- 5283-5283
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W3092926896
- Cited by
- 572
- References
- 83
- FWCI
- 12.96
- Type
- journal article
- Language
- en
- Open access
- gold
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- Marshall-Roth, T., Libretto, N. J., Wrobel, A. T., Anderton, K. J., Pegis, M. L., Ricke, N. D., Voorhis, T. V., Miller, J. T., & Surendranath, Y. (2020). A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts. Nature Communications. https://doi.org/10.1038/s41467-020-18969-6
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