Atomically dispersed iron sites with a nitrogen–carbon coating as highly active and durable oxygen reduction catalysts for fuel cells

Shengwen Liu, Chenzhao Li, Michael J. Zachman, Yachao Zeng, Haoran Yu, Boyang Li, Maoyu Wang, Jonathan Braaten, Jiawei Liu, Harry M. Meyer, Marcos Lucero, A. Jeremy Kropf, E. Ercan Alp, Qing Gong, Qiurong Shi, Zhenxing Feng, Hui Xu, Guofeng Wang (), Deborah J. Myers (), Jian Xie (), David A. Cullen (), Shawn Litster () and Gang Wu ()
Additional contact information
Shengwen Liu: University at Buffalo, The State University of New York
Chenzhao Li: Indiana University–Purdue University
Michael J. Zachman: Oak Ridge National Laboratory
Yachao Zeng: University at Buffalo, The State University of New York
Haoran Yu: Oak Ridge National Laboratory
Boyang Li: University of Pittsburgh
Maoyu Wang: Oregon State University Corvallis
Jonathan Braaten: Carnegie Mellon University
Jiawei Liu: Carnegie Mellon University
Harry M. Meyer: Oak Ridge National Laboratory
Marcos Lucero: Oregon State University Corvallis
A. Jeremy Kropf: Argonne National Laboratory
E. Ercan Alp: Argonne National Laboratory
Qing Gong: Indiana University–Purdue University
Qiurong Shi: University at Buffalo, The State University of New York
Zhenxing Feng: Oregon State University Corvallis
Hui Xu: Giner Inc.
Guofeng Wang: University of Pittsburgh
Deborah J. Myers: Argonne National Laboratory
Jian Xie: Indiana University–Purdue University
David A. Cullen: Oak Ridge National Laboratory
Shawn Litster: Carnegie Mellon University
Gang Wu: University at Buffalo, The State University of New York

Nature Energy, 2022, vol. 7, issue 7, 652-663

Abstract: Abstract Nitrogen-coordinated single atom iron sites (FeN4) embedded in carbon (Fe–N–C) are the most active platinum group metal-free oxygen reduction catalysts for proton-exchange membrane fuel cells. However, current Fe–N–C catalysts lack sufficient long-term durability and are not yet viable for practical applications. Here we report a highly durable and active Fe–N–C catalyst synthesized using heat treatment with ammonia chloride followed by high-temperature deposition of a thin layer of nitrogen-doped carbon on the catalyst surface. We propose that catalyst stability is improved by converting defect-rich pyrrolic N-coordinated FeN4 sites into highly stable pyridinic N-coordinated FeN4 sites. The stability enhancement is demonstrated in membrane electrode assemblies using accelerated stress testing and a long-term steady-state test (>300 h at 0.67 V), approaching a typical Pt/C cathode (0.1 mgPt cm−2). The encouraging stability improvement represents a critical step in developing viable Fe–N–C catalysts to overcome the cost barriers of hydrogen fuel cells for numerous applications.

Date: 2022
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DOI: 10.1038/s41560-022-01062-1

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