Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction

Abstract

The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N₄, accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

Graphical abstract

Keywords

oxygen reduction reaction / Fe-N-C / active sites / Fe addition / second heat treatment

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Acknowledgment

This work was funded by the National Natural Science Foundation of China (Grant Nos. 21533005 and 21802095) and the National Key R&D Program of China (2016YFB0101201).

Electronic Supplementary Material

ƒSupplementary material is available in the online version of this article at https://doi.org/10.1007/s11708-020-0669-0 and is accessible for authorized users.

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