Versatile Strategy for Tuning ORR Activity of a Single Fe-N-4 Site by Controlling Electron-Withdrawing/Donating Properties of a Carbon Plane

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Replacement of Pt-based oxygen reduction reaction (ORR) catalysts with non-precious metal catalysts (NPMCs) such as Fe/N/C is one of the most important issues in the commercialization of proton exchange membrane fuel cells (PEMFCs). Despite numerous studies on Fe/N/C catalysts, a fundamental study on the development of a versatile strategy is still required for tuning the kinetic activity of a single Fe-N-4 site. Herein, we report a new and intuitive design strategy for tuning and enhancing the kinetic activity of a single Fe-N-4 site by controlling electron-withdrawing/donating properties of a carbon plane with the incorporation of sulfur functionalities. The effect of electron-withdrawing/donating functionalities was elucidated by experimentation and theoretical calculations. Finally, the introduction of an oxidized sulfur functionality decreases the d-band center of iron by withdrawing electrons, thereby facilitating ORR at the Fe-N-4 site by lowering the intermediate adsorption energy. Furthermore, this strategy can enhance ORR. activity without a decrease in the stability of the catalyst. This simple and straightforward approach can be a cornerstone to develop optimum NPMCs for application in the cathodes of PEMFCs.
Publisher
AMER CHEMICAL SOC
Issue Date
2019-04
Language
English
Article Type
Article
Citation

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.141, no.15, pp.6254 - 6262

ISSN
0002-7863
DOI
10.1021/jacs.8b13543
URI
http://hdl.handle.net/10203/261871
Appears in Collection
CBE-Journal Papers(저널논문)
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