Versatile Strategy for Tuning ORR Activity of a Single Fe-N-4 Site by Controlling Electron-Withdrawing/Donating Properties of a Carbon Plane
SCIE
SCOPUS
- Title
- Versatile Strategy for Tuning ORR Activity of a Single Fe-N-4 Site by Controlling Electron-Withdrawing/Donating Properties of a Carbon Plane
- Authors
- Mun, Yeongdong; LEE, SEONG GYU; KIM, KYEOUNGHAK; KIM, SEONGBEEN; LEE, SEUNGHYUN; HAN, JEONG WOO; LEE, JIN WOO
- Date Issued
- 2019-04
- Publisher
- AMER CHEMICAL SOC
- Abstract
- 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.
- URI
- https://oasis.postech.ac.kr/handle/2014.oak/98664
- DOI
- 10.1021/jacs.8b13543
- ISSN
- 0002-7863
- Article Type
- Article
- Citation
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, vol. 141, no. 15, page. 6254 - 6262, 2019-04
- Files in This Item:
- There are no files associated with this item.
Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.