Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.077
Publication date: 18th July 2023
Pyrolized iron-based catalysts are one of the most promising alternatives to platinum, for the oxygen reduction reaction (ORR) taking place at the cathode of fuel cells. However, the pyrolysis step leads to the formation of a plethora of iron sites. Characterizing these sites under reaction conditions is challenging, and thus complicates fundamental studies of the catalyst. In turn, this hinders the rational optimization of pyrolized Fe-based catalysts.
On the other hand, iron macrocycles, with their well-defined structures, offer a platform for the study of the oxygen reduction reaction on FeN4 active sites. These macrocycles exhibit one or two distinctive peaks in their cyclic voltammograms, the origin of which is still debated. There have also been reports suggesting that the position of the high-potential peak correlates with the activity of the motif, making it a powerful performance descriptor and a tool to obtain structure-property relationships of FeN4 sites.
in this study, several iron macrocycles with different ligands and active sites were investigated, using electrochemistry, operando optical spectroscopy and DFT simulations. Optical spectroscopy results (shown in the TOC for the molecule FePC) show potential-dependent spectral changes in concomitance with the CV peaks. This, with the help DFT simulations, allowed us to identify the origin of the spectral change and to propose the existence of two families of macrocycles, with drastically different ORR activity. One group is characterized by two CV peaks, high ORR activity and low peroxide yield, while the other features a single CV peak, poor catalytic performance and higher peroxide production.
This study provides a first step in understanding what controls the activity of FeN4 sites and offers a tool to unravel fundamental properties of pyrolized FeNx catalysts.
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