High loading of single atomic iron sites in Fe-NC oxygen reduction catalysts for proton exchange membrane fuel cells
File(s)Fe-NC manuscript_Nature Catalysis_R4.docx (13.83 MB) Fe-NC_suppl information_Nature Catalysis_R4.pdf (2.97 MB)
Accepted version
Supporting information
Author(s)
Type
Journal Article
Abstract
Non-precious iron-based catalysts (Fe-NCs) require high active site density (SD) to meet the performance targets as cathode catalysts in proton exchange membrane fuel cells (PEMFCs). SD is generally limited to that achieved at 1-3 wt%(Fe) loading due to the undesired formation of iron-containing nanoparticles at higher loadings. Here we show that by pre-forming a carbon-nitrogen matrix using a sacrificial metal (Zn) in the initial synthesis step and then exchanging iron into this preformed matrix we achieve 7 wt% iron coordinated solely as single atom Fe-N4 sites as identified by 57Fe cryo Mössbauer spectroscopy and X-ray absorption spectroscopy. SD values measured by in situ nitrite stripping and ex situ CO chemisorption methods are 4.7x1019 and 7.8x1019 sitesg-1, with a turnover frequency of 5.4 electrons̭sites-1s-1 at 0.80 V in 0.5M H2SO4 electrolyte. The catalyst delivers excellent PEMFC performance with current densities of 41.3 mAcm-2 at 0.90 ViR-free using H2-O2 (10.6 Ag-1) and 145 mA cm-2 at 0.80 V (199 mAcm-2 at 0.80 ViR-free) using H2-air.
Date Issued
2022-04-25
Date Acceptance
2022-03-11
Citation
Nature Materials, 2022, 5, pp.311-323
ISSN
1476-1122
Publisher
Nature Research
Start Page
311
End Page
323
Journal / Book Title
Nature Materials
Volume
5
Copyright Statement
© The Author(s), under exclusive licence to Springer Nature Limited 2022. The final publication is available at Springer via https://doi.org/10.1038/s41929-022-00772-9
Sponsor
Engineering & Physical Science Research Council (E
Commission of the European Communities
Identifier
https://www.nature.com/articles/s41929-022-00772-9
Grant Number
EP/P024807/1
779366
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
RAY-ABSORPTION SPECTROSCOPY
BODY DISTRIBUTION-FUNCTIONS
NITROGEN-CARBON CATALYSTS
ACTIVE-SITES
DOPED CARBON
TURNOVER FREQUENCY
CONDENSED MATTER
C CATALYSTS
METAL
PERFORMANCE
Publication Status
Published
Date Publish Online
2022-04-25