期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 3, 期 4, 页码 1752-1760出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4ta03986f
关键词
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资金
- Danish ForskEL (Catbooster)
- Danish Council for Strategic Research (4M Centre)
- National Basic Research Program of China (973 Program) [2012CB215500]
- National High Technology Research and Development Program of China (863 Program) [2012AA053401]
We present a detailed study of a novel Fe3C-based spherical catalyst with respect to synthetic parameters, nanostructure formation, ORR active sites and fuel cell demonstration. The catalyst is synthesized by high-temperature autoclave pyrolysis using decomposing precursors. Below 500 degrees C, melamine-rich microspheres are first developed with uniformly dispersed amorphous Fe species. During the following pyrolysis at temperatures from 600 to 660 degrees C, a small amount of Fe3C phase with possible Fe-N-x/C active sites are formed, however, with moderate catalytic activity, likely limited by the low conductivity of the catalyst. At high pyrolytic temperatures of 700-800 degrees C, simultaneous formation of Fe3C nanoparticles and encasing graphitic layers occur within the morphological confinement of the microspheres. With negligible surface nitrogen or iron functionality, the thus-obtained catalysts exhibit superior ORR activity and stability. A new ORR active phase of Fe3C nanoparticles encapsulated by thin graphitic layers is proposed. The activity and durability of the catalysts are demonstrated in both Nafion-based low temperature and acid doped polybenzimidazole-based high temperature proton exchange membrane fuel cells.
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