期刊
NATURE ENERGY
卷 7, 期 7, 页码 652-663出版社
NATURE PORTFOLIO
DOI: 10.1038/s41560-022-01062-1
关键词
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资金
- US DOE Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office [DE-EE0008076, DE-EE0008417]
- Center for Nanophase Materials Sciences (CNMS), US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory
- US DOE by the University of Chicago Argonne LLC [DE-AC02-06CH11357]
- National Science Foundation [CBET-1949870, 2016192]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [2016192] Funding Source: National Science Foundation
In this study, a highly durable and active Fe-N-C catalyst was synthesized by depositing a thin layer of nitrogen-doped carbon on the catalyst surface. The stability improvement of the catalyst can overcome the cost barriers of hydrogen fuel cells.
Fe-N-C materials are promising oxygen reduction catalysts for proton-exchange membrane fuel cells but still lack sufficient long-term durability for practical applications. Here the authors fabricate an Fe-N-C material with a thin N-C layer on the surface, leading to a highly durable and active catalyst. 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 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.
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