Authors
Yachao Zeng, Chenzhao Li, Boyang Li, Jiashun Liang, Michael J Zachman, David A Cullen, Raphael P Hermann, E Ercan Alp, Barbara Lavina, Stavros Karakalos, Marcos Lucero, Bingzhang Zhang, Maoyu Wang, Zhenxing Feng, Guofeng Wang, Jian Xie, Deborah J Myers, Jean-Pol Dodelet, Gang Wu
Publication date
2023/12
Journal
Nature Catalysis
Volume
6
Issue
12
Pages
1215-1227
Publisher
Nature Publishing Group UK
Description
Fe–N–C catalysts are the most promising platinum group metal-free oxygen-reduction catalysts, but they suffer from a low density of active metal sites and the so-called activity–stability trade-off. Here we report an Fe–N–C catalyst prepared by adding an optimal amount of H2 to the traditional inert atmosphere during the thermal activation. The presence of H2 significantly increases the total density of FeN4 sites, suppressing the unstable pyrrolic-N-coordinated S1 sites and favouring the stable pyridinic-N-coordinated S2 sites with shortened Fe–N bond lengths. We propose that the intrinsically stable S2 sites are probably arranged in well-graphitized carbon layers, and the S1 sites exist in less-graphitized carbon. H2 could remove unstable S1 sites and retain stable S2 sites during the pyrolysis to break the challenging activity–stability trade-off. The Fe–N–C catalyst in membrane electrode assemblies maintains a …
Total citations
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