Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 26, Issue 31, Pages 5708-5717Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201601492
Keywords
iron; nitrogen-doped graphene; oxygen reduction reaction; pyridinic nitrogen
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Funding
- National Basic Research Program of China (973 program) [2013CB934301]
- National Natural Science Foundation of China [51531006, 51572148, 51572007]
- Research Project of Chinese Ministry of Education [113007A]
- Tsinghua University Initiative Scientific Research Program
- U.S. Air Force Office of Scientific Research 3D MURI Award [FA9550-12-1-0035]
- Fundamental Research Funds for the Central Universities [YWF-16-BJ-Y-12]
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Here, pyridinic nitrogen dominated graphene aerogels with/without iron incorporation (Fe-NG and NG) are prepared via a facile and effective process including freeze-drying of chemically reduced graphene oxide with/without iron precursor and thermal treatment in NH3. A high doping level of nitrogen has been achieved (up to 12.2 at% for NG and 11.3 at% for Fe-NG) with striking enrichment of pyridinic nitrogen (up to 90.4% of the total nitrogen content for NG, and 82.4% for Fe-NG). It is found that the Fe-NG catalysts display a more positive onset potential, higher current density, and better four-electron selectivity for ORR than their counterpart without iron incorporation. The most active Fe-NG exhibits outstanding ORR catalytic activity, high durability, and methanol tolerance ability that are comparable to or even superior to those of the commercial Pt/C catalyst at the same catalyst loading in alkaline environment. The excellent ORR performance can be ascribed to the synergistic effect of pyridinic N and Fe-N (x) sites (where iron probably coordinates with pyridinic N) that serve as active centers for ORR. Our Fe-NG can be developed into cost-effective and durable catalysts as viable replacements of the expensive Pt-based catalysts in practical fuel cell applications.
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