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

Liu, Shengwen; Li, Chenzhao; Zachman, Michael J.; Zeng, Yachao; Yu, Haoran; Li, Boyang; Wang, Maoyu; Braaten, Jonathan; Liu, Jiawei; Meyer, III, Harry M.; Lucero, Marcos; Kropf, A. Jeremy; Alp, E. Ercan; Gong, Qing; Shi, Qiurong; Feng, Zhenxing; Xu, Hui; Wang, Guofeng; Myers, Deborah J.; Xie, Jian; Cullen, David A.; Litster, Shawn; Wu, Gang

doi:10.1038/s41560-022-01062-1

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

Journal Article · Thu Jul 07 00:00:00 EDT 2022 · Nature Energy

DOI:https://doi.org/10.1038/s41560-022-01062-1· OSTI ID:1881116

Liu, Shengwen ^[1]; Li, Chenzhao ^[2]; ^[3]; Zeng, Yachao ^[1]; ^[3]; Li, Boyang ^[4]; Wang, Maoyu ^[5]; Braaten, Jonathan ^[6]; ^[6]; ^[7]; ^[5]; ^[8]; Alp, E. Ercan ^[9]; Gong, Qing ^[10]; Shi, Qiurong ^[1]; ^[5]; Xu, Hui ^[11]; ^[4]; ^[8]; ^[10] more »

State Univ. of New York (SUNY), Buffalo, NY (United States)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Purdue Univ., West Lafayette, IN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Pittsburgh, PA (United States)
Oregon State Univ., Corvallis, OR (United States)
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
Giner, Inc., Newton, MA (United States)

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. Still, 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 mg_Pt 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Nuclear Energy (NE), Nuclear Fuel Cycle and Supply Chain. Fuel Cycle Research and Development Program; National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; EE0008076; EE0008417; AC02-06CH11357

OSTI ID:: 1881116

Alternate ID(s):: OSTI ID: 1897111
OSTI ID: 1969732

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 7 Vol. 7; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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