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Chemical vapor deposition of Fe-N-C oxygen reduction catalysts with full utilization of dense Fe-N4 sites.pdf (2.43 MB)
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Chemical Vapor Deposition of Fe-N-C Oxygen Reduction Catalysts with Full Utilization of Dense Fe-N4 Sites

preprint
submitted on 04.09.2020 and posted on 07.09.2020 by Li Jiao, Jingkun Li, Lynne Larochelle Richard, Qiang Sun, Thomas Stracensky, Ershuai Liu, Moulay-Tahar Sougrati, Zipeng Zhao, Fan Yang, Sichen Zhong, Hui Xu, Sanjeev Mukerjee, Yu Huang, David A Cullen, Deborah J. Myers, Frederic Jaouen, Qingying Jia
Replacing scarce and expensive platinum (Pt) with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) has largely been impeded by the low activity of M-N-C, in turn limited by low site density and low site utilization. Herein, we overcome these limits by implementing chemical vapor deposition (CVD) to synthesize Fe-N-C, an approach fundamentally different from previous routes. The Fe-N-C catalyst, prepared by flowing iron chloride vapor above a N-C substrate at 750 ℃, has a record Fe-N4 site density of 2×1020 sites·gram-1 with 100% site utilization. A combination of characterizations shows that the Fe-N4 sites formed via CVD are located exclusively on the outer-surface, accessible by air, and electrochemically active. This catalyst delivers an unprecedented current density of 33 mA·cm-2 at 0.90 ViR-free (iR-corrected) in an H2-O2 PEMFC at 1.0 bar and 80 ℃.

Funding

US Department of Energy under award number DE-EE0008416 and DE-EE0008075.

History

Email Address of Submitting Author

jiao.li@northeastern.edu

Institution

Northeastern Univeristy

Country

美国

ORCID For Submitting Author

0000-0002-1063-9313

Declaration of Conflict of Interest

L.J., S.M., and Q.J. have filed a provisional patent (NO. 62/945,861) application based on the results of this manuscript.

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