Electronic Structure and Reaction Mechanism on Nitrogen-doped Carbon Electrode Catalysts and Design of Catalyst Based on the Mechanism

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  • TAKEYASU Kotaro
    Faculty of Faculty of Pure and Applied Sciences, University of Tsukuba Tsukuba Research Centre for Energy and Materials Science, University of Tsukuba R&D Center for Zero CO<sub>2</sub> Emission with Functional Materials, University of Tsukuba
  • NAKAMURA Junji
    Tsukuba Research Centre for Energy and Materials Science, University of Tsukuba Mitsui Chemicals, Inc. - Carbon Neutral Research Center (MCI-CNRC), International Institute for Carbon-Neutral Energy Research (I<sup>2</sup>CNER), Kyushu University

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  • 窒素ドープカーボン電極触媒の電子状態と反応機構，それに基づく触媒設計
  • チッソ ドープカーボン デンキョク ショクバイ ノ デンシ ジョウタイ ト ハンノウ キコウ,ソレニ モトズク ショクバイ セッケイ

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Abstract

<p>Nitrogen-doped carbons are plausible candidates for alternative catalysts of platinum-based catalysts for oxygen reduction reaction (ORR). Although nitrogen-doped carbons are highly active in alkaline media, the activities critically decrease under acidic conditions in fuel cells. To overcome the problem, we have investigated the reaction mechanism based on the electronic structures by using model catalysts. On the active site of pyridinic nitrogen (pyri-N), we have reported that O2＋pyri-NH＋＋e－→O2a＋pyri-NH governs the ORR activities, where the adsorbed O2 make a bond with an electron doped into π* orbital of the carbons. In the elementary step, the hydration of pyri-NH＋ decreases the redox potential and resultantly the ORR activity. Therefore, we designed a nitrogen-doped graphene catalysts with higher hydrophobicity to prevent the hydration. To compensate the decreased conductivity, we introduced a proton-conductive particles. Thus, the compatible hydrophobicity and proton conductivity achieved the highest activity as a metal-free ORR catalyst.</p>

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