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Niwa, Hideharu*; Saito, Makoto*; Kobayashi, Masaki*; Harada, Yoshihisa*; Oshima, Masaharu*; Moriya, Shogo*; Matsubayashi, Katsuyuki*; Nabae, Yuta*; Kuroki, Shigeki*; Ikeda, Takashi; et al.
Journal of Power Sources, 223, p.30 - 35, 2013/02
Times Cited Count：18 Percentile：49.15(Chemistry, Physical)To design non-platinum, inexpensive, but high performance carbon-based cathode catalysts for polymer electrolyte fuel cells, it is important to elucidate the active site for oxygen reduction reaction (ORR). However, it is difficult to directly identify the active site by applying conventional structural or electronic probes to such complex systems. Here, we used C 1
X-ray absorption spectroscopy (XAS) to observe electronic structure of carbon in iron phthalocyanine-based catalysts, and found a signature of edge exposure below the 
edge, whose intensity is well correlated with the ORR activity. These results demonstrate that C 1 XAS can be used to characterize the ORR activity of carbon-based cathode catalysts in terms of the edge exposure.
Kiuchi, Hisao*; Niwa, Hideharu*; Kobayashi, Masaki*; Harada, Yoshihisa*; Oshima, Masaharu*; Chokai, Masayuki*; Nabae, Yuta*; Kuroki, Shigeki*; Kakimoto, Masaaki*; Ikeda, Takashi; et al.
Electrochimica Acta, 82(1), p.291 - 295, 2012/10
Times Cited Count：14 Percentile：33.07(Electrochemistry)We study the characteristics of oxygen adsorption on metal-free carbon-based cathode catalysts derived from nitrogen-containing polyamide (PA) and nitrogen-free phenolic resin (PhRs). Electrochemical analysis and Raman spectroscopy showed higher 2-electron oxygen reduction reaction (ORR) activity and more defect sites in PA than PhRs. The increase in the amount of adsorbed oxygen in PA was also identified by oxygen adsorption isotherms. 
X-ray photoelectron spectroscopy reveals that graphite-like nitrogen contributes to oxygen adsorption and C=O components are dominant in PA. These experimental results indicate that the adsorbed C=O components near the graphite-like nitrogen can be assigned as active sites for 2-electron ORR.
