X-ray photoemission spectroscopy analysis of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells

被引:90
作者
Niwa, Hideharu [1 ]
Kobayashi, Masaki [1 ,2 ]
Horiba, Koji [1 ,2 ]
Harada, Yoshihisa [1 ,2 ]
Oshima, Masaharu [1 ,2 ]
Terakura, Kiyoyuki [3 ]
Ikeda, Takashi [4 ]
Koshigoe, Yuka [5 ]
Ozaki, Jun-ichi [5 ]
Miyata, Seizo [6 ]
Ueda, Shigenori [7 ]
Yamashita, Yoshiyuki [7 ]
Yoshikawa, Hideki [7 ]
Kobayashi, Keisuke [7 ]
机构
[1] Univ Tokyo, Sch Engn, Dept Appl Chem, Bunkyo Ku, Tokyo 1138656, Japan
[2] Univ Tokyo, Synchrotron Radiat Res Org, Bunkyo Ku, Tokyo 1138656, Japan
[3] JAIST, Res Ctr Integrated Sci, Nomi Ishikawa 9231292, Japan
[4] JAEA, Quantum Beam Sci Directorate, Sayo, Hyogo 6795148, Japan
[5] Gunma Univ, Grad Sch Engn, Dept Chem & Environm Engn, Gunma 3768515, Japan
[6] New Energy & Ind Technol Dev Org, Saiwai Ku, Kanagawa 2128554, Japan
[7] NIMS, Sayo, Hyogo 6795148, Japan
关键词
Polymer electrolyte fuel cell; Cathode; Oxygen reduction reaction; X-ray photoemission spectroscopy; Carbon alloy catalysts; Electronic structure; OXYGEN-REDUCTION ACTIVITY; COMPOSITE CATALYSTS; HEAT-TREATMENT; ACTIVE-SITES; ENHANCEMENT; ABSORPTION; FE; COMPLEXES; GRAPHITE; SPECTRA;
D O I
10.1016/j.jpowsour.2010.08.054
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We report on the electronic structure of three different types of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells observed by hard X-ray photoemission spectroscopy. Prepared samples are derived from: (1) melamine and poly(furfuryl alcohol), (2) nitrogen-doped carbon black and (3) cobalt phthalocyanine and phenolic resin. C 1s spectra show the importance of sp(2) carbon network formation for the oxygen reduction reaction (ORR) activity. N 1s spectra of the carbon-based cathode catalysts are decomposed into four components identified as pyridine-like, pyrrole- or cyanide-like, graphite-like, and oxide nitrogen. Samples having high oxygen reduction reaction activity in terms of oxygen reduction potential contain high concentration of graphite-like nitrogen. O 1s spectra are similar among carbon-based cathode catalysts of different oxygen reduction reaction activity. There is no correlation between the ORR activity and oxygen content. Based on a quantitative analysis of our results, the oxygen reduction reaction activity of the carbon-based cathode catalysts will be improved by increasing concentration of graphite-like nitrogen in a developed sp(2) carbon network. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:1006 / 1011
页数:6
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