期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 52, 页码 18971-18980出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201909312
关键词
electrode materials; iron; nanomaterials; oxygen reduction reaction; proton-exchange membrane fuel cells
资金
- National Science Foundation (NSF) [CBET-1604392, 1804326]
- U.S. Department of Energy, Fuel Cell Technologies Office [DE-EE0008076]
- NSF [CBET-804534, ACI-1053575]
- Argonne National Laboratory [DE-AC02-06CH11357]
- E. I. duPont de Nemours Co.
- Northwestern University
- Dow Chemical Company
- National Natural Science Foundation of China [21273058, 21673064]
FeN4 moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton-exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe-N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high-temperature treatment. Here, we elucidate the FeN4 site formation mechanisms through hosting Fe ions into a nitrogen-doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF-8-derived nitrogen-doped carbon is an ideal model with well-defined nitrogen doping and porosity. This approach is able to deconvolute Fe-N bond formation from complex carbonization and nitrogen doping, which correlates Fe-N bond properties with the activity and stability of FeN4 sites as a function of the thermal activation temperature.
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