Development of a highly active Fe-N-C catalyst with the preferential formation of atomic iron sites for oxygen reduction in alkaline and acidic electrolytes
File(s)Highlighted Revision.docx (16.61 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
Nitrogen-doped porous carbons containing atomically dispersed iron are prime candidates for substituting platinum-based catalysts for oxygen reduction reaction (ORR) in fuel cells. These carbon catalysts are classically synthesized via complicated routes involving multiple heat-treatment steps to form the desired Fe-Nx sites. We herein developed a highly active Fesingle bondNsingle bondC catalyst comprising of exclusive Fe-Nx sites by a simplified solid-state synthesis protocol involving only a single heat-treatment. Imidazole is pyrolyzed in the presence of an inorganic salt-melt resulting in highly porous carbon sheets decorated with abundant Fe-Nx centers, which yielded a high density of electrochemically accessible active sites (1.36 × 1019 sites g−1) as determined by the in situ nitrite stripping technique. The optimized catalyst delivered a remarkable ORR activity with a half-wave potential (E1/2) of 0.905 VRHE in alkaline electrolyte surpassing the benchmark Pt catalyst by 55 mV. In acidic electrolyte, an E1/2 of 0.760 VRHE is achieved at a low loading level (0.29 mg cm−2). In PEMFC tests, a current density of 2.3 mA cm−2 is achieved at 0.90 ViR-free under H2–O2 conditions, reflecting high kinetic activity of the optimized catalyst.
Date Issued
2021-08-15
Date Acceptance
2021-03-14
Citation
Journal of Colloid and Interface Science, 2021, 596, pp.148-157
ISSN
0021-9797
Publisher
Elsevier
Start Page
148
End Page
157
Journal / Book Title
Journal of Colloid and Interface Science
Volume
596
Copyright Statement
© 2021 Elsevier Ltd. All rights reserved. This manuscript is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International Licence http://creativecommons.org/licenses/by-nc-nd/4.0/
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000645630200002&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
Non-precious metal catalysts
Fe-N-C
Fuel cells
Oxygen reduction reaction
Site density
METAL ELECTROCATALYST
CARBON
PERFORMANCE
POLYANILINE
EFFICIENT
ELECTROREDUCTION
MELAMINE
DENSITY
FE/N/C
STABILITY
Publication Status
Published
Date Publish Online
2021-03-19