Journal
ADVANCED MATERIALS INTERFACES
Volume 8, Issue 8, Pages -Publisher
WILEY
DOI: 10.1002/admi.202001788
Keywords
controllable and scalable synthesis; Fe single‐ atom catalysts; FeN4 active center; oxygen reduction reaction
Funding
- Australian Research Council Discovery Project Funding Scheme [DP180100568, DP180100731]
- University of Western Australia - Australian Research Council LIEF grant [LE120100026]
- National Natural Science Foundation of China [51521091, 51872293]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering
- ORNL's Center for Nanophase Materials Sciences
- Scientific User Facilities Division of U.S. Department of Energy
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This study demonstrates a scalable method for synthesizing single atom iron catalysts, in which iron atoms are coordinated with nitrogen on graphene through a pyrolysis process, resulting in a high atomic loading catalyst. The Fe-N-G catalyst exhibits high performance and microstructure stability in the ORR process, with FeN4 confirmed as the active center.
Single atom catalysts (SACs) have attracted much attentions due to their advantages of high catalysis efficiency and excellent selectivity. However, for industrial applications, synthesis of SACs in large and practical quantities is very important. The challenge is to develop synthesis methods with controllability and scalability. Herein, a well-characterized and scalable method is demonstrated to synthesize atomically dispersed iron atoms coordinated with nitrogen on graphene, SAFe @ NG, with high atomic loading (approximate to 4.6 wt%) through a one-pot pyrolysis process. The method is scalable for the fabrication of Fe SACs with high quantities. The Fe-N-G catalyst exhibits high intrinsic oxygen reduction reaction (ORR) performance, reaching half potential of 0.876 and 0.702 V in alkaline and acidic solutions, respectively, with excellent microstructure stability. Furthermore, the density functional theory (DFT) simulation confirms that the Fe atoms in coordination with four nitrogen atoms, FeN4, in graphene is the active center for the 4-electron ORR process. This work demonstrates an efficient design pathway for single atom catalysts as highly active and stable electrocatalysts for high-performance ORR applications.
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