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X-ray absorption analysis of nitrogen contribution to oxygen reduction reaction in carbon alloy cathode catalysts for polymer electrolyte fuel cells

X線吸収による固体高分子形燃料電池用カーボンアロイカソード触媒での酸素還元反応に対する窒素の寄与の解析

丹羽 秀治*; 堀場 弘司*; 原田 慈久*; 尾嶋 正治*; 池田 隆司; 寺倉 清之*; 尾崎 純一*; 宮田 清蔵*

Niwa, Hideharu*; Horiba, Koji*; Harada, Yoshihisa*; Oshima, Masaharu*; Ikeda, Takashi; Terakura, Kiyoyuki*; Ozaki, Junichi*; Miyata, Seizo*

固体高分子形燃料電池のための炭素ベースのカソード触媒に導入された窒素の電子構造をX線吸収分光法を用いて調べた。N 1s吸収スペクトルにおけるプレエッジ領域の$$pi^{ast}$$ピークの形状は窒素の化学状態の決定に用いることができ、酸素還元活性の指標として用いることができる。高活性な触媒はピリジン様窒素よりもグラファイト様窒素を比較的多く含むことがわかった。

The electronic structure of nitrogens introduced in various carbon-based cathode catalysts for a polymer electrolyte fuel cell (PEFC) has been investigated using X-ray absorption spectroscopy (XAS). The profile of the $$pi^{ast}$$ peaks at the pre-edge of the N 1s XAS spectra is used to determine the chemical states of nitrogens, which can be a marker of the oxygen reduction reaction (ORR) activity; it is found that catalysts that have relatively high amount of graphite-like nitrogen exhibit higher ORR activity than those having relatively high amount of pyridine-like nitrogen. We propose that effective doping of graphite-like nitrogen is a practical guideline for the synthesis of active carbon alloy catalysts.

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パーセンタイル:99.83

分野:Chemistry, Physical

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