Chemical vapour deposition of Fe-N-C oxygen reduction catalysts with full utilization of dense Fe-N4 sites.

Nature Materials
Li JiaoQingying Jia

Abstract

Replacing scarce and expensive platinum (Pt) with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has largely been impeded by the low oxygen reduction reaction activity of M-N-C due to low active site density and site utilization. Herein, we overcome these limits by implementing chemical vapour deposition to synthesize Fe-N-C by flowing iron chloride vapour over a Zn-N-C substrate at 750 °C, leading to high-temperature trans-metalation of Zn-N4 sites into Fe-N4 sites. Characterization by multiple techniques shows that all Fe-N4 sites formed via this approach are gas-phase and electrochemically accessible. As a result, the Fe-N-C catalyst has an active site density of 1.92 × 1020 sites per gram with 100% site utilization. This catalyst delivers an unprecedented oxygen reduction reaction activity of 33 mA cm-2 at 0.90 V (iR-corrected; i, current; R, resistance) in a H2-O2 proton exchange membrane fuel cell at 1.0 bar and 80 °C.

References

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Jul 25, 2012·Physical Chemistry Chemical Physics : PCCP·Ulrike I KrammJean-Pol Dodelet
Oct 22, 2015·Nature Communications·Nastaran Ranjbar SahraiePeter Strasser
Sep 14, 2017·Journal of the American Chemical Society·Hanguang ZhangGang Wu
Feb 19, 2019·Advanced Materials·Ulrike I KrammStephan Wagner
Feb 20, 2019·Advanced Materials·Yuyan ShaoPiotr Zelenay
Dec 28, 2019·Journal of the American Chemical Society·Jingkun LiQingying Jia

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