期刊
CARBON
卷 78, 期 -, 页码 49-59出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2014.06.047
关键词
-
资金
- National Natural Science Foundation [21303058]
- Shanghai Municipal Natural Science Foundation [13ZR1412400]
- Shanghai Science and Technology Committee [11JC1403400]
Novel mesoporous Fe (or Co)-N-x-C non-precious-metal catalysts (NPMCs) have been fabricated by a simple nanocasting-pyrolysis method using 1,10-phenanthroline metal chelates as the precursors. Owing to the ordered hexagonal mesostructures, appropriate surface area, large-pore channels, and well-distributed metal-N-x moieties embedded within the graphitic carbon backbones, the prepared metal-N-x-C materials exhibit excellent catalytic activity for oxygen reduction reaction (ORR) in both alkaline and acidic media. The prepared Fe-N-x-C materials, when prepared with an optimized catalyst loading on the electrode, exhibit more positive ORR onset-potential and half-wave potential (E-1/2) than commercial Pt/C catalysts and the previously reported NPMCs in 0.1 M KOH electrolyte. They also have the comparable ORR onset-potential and current densities to Pt/C electrode in 0.1 M HClO4 electrolyte. Moreover, ORR over mesoporous Fe-N-x-C was found to proceed by the direct four-electron mechanism with high selectivity in both electrolytes. The mesoporous Fe-N-x-C materials demonstrated higher ORR catalytic activity compared to the NPMCs made by alternative methods. Analysis of the catalytic behavior, structure and nature of surface species of N-x-C materials allows us to ascribe the origin of the excellent ORR catalytic activity of mesoporous Fe (or Co)-N-x-C in both electrolytes to Fe (or Co)-N-x moieties embedded within the graphitic carbon frameworks. (C) 2014 Elsevier Ltd. All rights reserved.
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