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Stabilizing Single-Atom Iron Electrocatalysts for Oxygen Reduction via Ceria Confining and Trapping

Journal Article · · ACS Catalysis
 [1];  [2];  [2];  [3];  [4];  [5];  [5];  [5];  [5];  [6]
  1. Hong Kong Univ. of Science and Technology, Guangzhou (China); Washington State Univ., Pullman, WA (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry ; Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry
  5. Washington State Univ., Pullman, WA (United States)
  6. Hong Kong Univ. of Science and Technology, Guangzhou (China)
+ Show Author Affiliations
Atomically dispersed Fe-N-C materials recently hold great interest in costly Pt substitution for the cathodic oxygen reduction reaction of fuel cells. However, the heat treatment involved in the materials preparation excites Fe aggregating into low activity of nanosized species rather than high activity of single-atom Fe sites. Herein we proposed a new "ceria-assisted" strategy to preferentially generate the active single-atom Fe sites in Fe-N-C materials, which involves oxidative polymerization of pyrrole, Ce3+ and Fe3+ adsorption, and subsequent heat treatment. Owing to its spatial confinement and strong trapping for Fe atoms, ceria can effectively suppress agglomeration of isolated Fe atoms and stabilize the Fe atoms by bonding to O in the lattice during the heat treatment, leading to a high content of atomically dispersed Fe (4.6 wt.%). Accordingly, the final catalyst showed ultrahigh ORR activity with a half-wave potential of 0.915 V and kinetic current density of 7.15 mA cm-2 at 0.9 V. When it was as assembled an anion exchange membrane fuel cell, a large maximum power density of 496 mW cm-2 was achieved.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Organization:
National Key Research and Development Program of China
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1631589
Journal Information:
ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 4 Vol. 10; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Fe-N
anion exchange membrane fuel cell
ceria
oxygen reduction
single-atom catalysts