Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.270
Publication date: 11th July 2022
One of the major hindrances to mass commercialization of low-temperature proton-exchange-membrane fuel cells (PEMFCs) is the considerable amount of expensive Pt required, especially at the cathode side, where the oxygen reduction reaction (ORR) takes place.1, 2
In the last decade, great efforts have been made to develop efficient Platinum-Group-Metals (PGM) free catalysts for the ORR, especially metal-nitrogen-doped carbons (M-N-C, with M = Fe, Co), due to the abundance and inexpensiveness of their constituent elements and their atomic dispersion. The activity gap towards Pt has successfully been narrowed, now reaching the activity requirements for practical applications.3-5 Due to the metastability of the ORR active M-N4 sites at the temperature of their pyrolytic formation, the final transition metal loading is currently limited and significant amounts of inorganic by-products are formed. Although synthesis protocols have been successfully optimized, multiple processing steps are required, making the preparation time-consuming.
In our previous work, we showed that via an active-site imprinting strategy followed by a transmetalation reaction, Mg-N-C and Zn-N-C containing Mg-N4 and Zn-N4 sites respectively, can be transformed into active Fe-N-C electrocatalysts, avoiding the formation of elemental iron, or iron carbide side phases.6-8
In this work, we present how Zn−N4 sites in tailor-made Zn−N−C materials are utilized as an active-site imprint for the preparation of the corresponding Fe−N−C catalysts with a high loading of atomically dispersed Fe. The current state of this class of materials is discussed in terms of synthetic methods, activity and stability, including both rotating disk electrode (RDE) and single-cell PEMFC testing.
A. Kongkanand and M. F. Mathias, J. Phys. Chem. Lett., 2016, 7, 1127-1137.
S. T. Thompson and D. Papageorgopoulos, Nature Catalysis, 2019, 2, 558-561.
M. Lefèvre, E. Proietti, F. Jaouen and J.-P. Dodelet, Science, 2009, 324, 71-74.
R. Bashyam and P. Zelenay, Nature, 2006, 443, 63.
H. A. Gasteiger, S. S. Kocha, B. Sompalli and F. T. Wagner, Appl. Catal., B, 2005, 56, 9-3
A. Mehmood, J. Pampel, G. Ali, H. Y. Ha, F. Ruiz-Zepeda and T.-P. Fellinger, Advanced Energy Materials, 2018, 8, 1701771.
D. Menga, F. Ruiz-Zepeda, L. Moriau, M. Šala, F. Wagner, B. Koyutürk, M. Bele, U. Petek, N. Hodnik, M. Gaberšček and T.-P. Fellinger, Advanced Energy Materials, 2019, 9, 1902412.
8. D. Menga, J. L. Low, Y.-S. Li, I. Arčon, B. Koyutürk, F. Wagner, F. Ruiz-Zepeda, M. Gaberšček, B. Paulus and T.-P. Fellinger, Journal of the American Chemical Society, 2021, 143, 18010-18019.