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Title: Highly Graphitic Mesoporous Fe,N-Doped Carbon Materials for Oxygen Reduction Electrochemical Catalysts

Journal Article · · ACS Applied Materials and Interfaces

The synthesis, characterization, and electrocatalytic properties of mesoporous carbon materials doped with nitrogen atoms and iron are reported and compared for the catalyzed reduction of oxygen gas at fuel cell cathodes. Mixtures of common and inexpensive organic precursors, melamine, and formaldehyde were pyrolyzed in the presence of transition-metal salts (e.g., nitrates) within a mesoporous silica template to yield mesoporous carbon materials with greater extents of graphitization than those of others prepared from small-molecule precursors. In particular, Fe,N-doped carbon materials possessed high surface areas (~800 m2/g) and high electrical conductivities (~19 S/cm), which make them attractive for electrocatalyst applications. The surface compositions of the mesoporous Fe,N-doped carbon materials were postsynthetically modified by acid washing and followed by high-temperature thermal treatments, which were shown by X-ray photoelectron spectroscopy to favor the formation of graphitic and pyridinic nitrogen moieties. Such surface-modified materials exhibited high electrocatalytic oxygen reduction activities under alkaline conditions, as established by their high onset and half-wave potentials (1.04 and 0.87 V, respectively vs reversible hydrogen electrode) and low Tafel slope (53 mV/decade). These values are superior to many similar transition-metal- and N-doped carbon materials and compare favorably with commercially available precious-metal catalysts, e.g., 20 wt % Pt supported on activated carbon. As a result, the analyses indicate that inexpensive mesoporous Fe,N-doped carbon materials are promising alternatives to precious metal-containing catalysts for electrochemical reduction of oxygen in polymer electrolyte fuel cells.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
U.S. Army; USDOE
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1542826
Report Number(s):
LA-UR-18-26362
Journal Information:
ACS Applied Materials and Interfaces, Vol. 10, Issue 30; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 40 works
Citation information provided by
Web of Science

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