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Incorporation of Multinuclear Copper Active Sites into Nitrogen-Doped Graphene for Electrochemical Oxygen Reduction

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Title: Incorporation of Multinuclear Copper Active Sites into Nitrogen-Doped Graphene for Electrochemical Oxygen Reduction
Authors: Kato, Masaru Browse this author →KAKEN DB
Muto, Marika Browse this author
Matsubara, Naohiro Browse this author
Uemura, Yohei Browse this author →KAKEN DB
Wakisaka, Yuki Browse this author
Yoneuchi, Tsubasa Browse this author
Matsumura, Daiju Browse this author →KAKEN DB
Ishihara, Tomoko Browse this author
Tokushima, Takashi Browse this author →KAKEN DB
Noro, Shin-ichiro Browse this author →KAKEN DB
Takakusagi, Satoru Browse this author →KAKEN DB
Asakura, Kiyotaka Browse this author →KAKEN DB
Yagi, Ichizo Browse this author →KAKEN DB
Keywords: Oxygen reduction reaction
Polymer electrolyte fuel cell
Nitrogen-doped graphene
Issue Date: 29-May-2018
Publisher: American Chemical Society
Journal Title: ACS Applied Energy Materials
Volume: 1
Issue: 5
Start Page: 2358
End Page: 2364
Publisher DOI: 10.1021/acsaem.8b00491
Abstract: Multinuclear metal active sites are widely used as catalytic reaction centers in metalloenzymes and generally show high catalytic activity. For example, laccases are known to catalyze the oxygen reduction reaction (ORR) to water at a multinuclear copper site with almost no energy loss. The ORR is an important reaction not only in oxygenic respiration but also in future energy generation devices such as polymer electrolyte fuel cells and metal–air batteries. For large-scale commercialization of these devices, there is a need to develop highly active ORR electrocatalysts based on non-precious metals. Incorporation of multinuclear metal active sites in conductive materials such as carbon will allow us to develop highly active electrocatalysts like metalloenzymes. However, such methods had not been established yet. Herein, we report a copper-based ORR electrocatalysts with multinuclear copper active sites in nitrogen-doped graphene. The electrocatalyst was synthesized from the mixture of graphene oxide and a multinuclear copper complex in a short-period heating method. Electrochemical measurements revealed that the obtained electrocatalyst showed the highest electrocatalytic activity for the ORR in the Cu-based electrocatalysts in neutral aqueous solution. Physicochemical measurements including in situ X-ray absorption spectroscopy revealed the incorporation of multinuclear copper sites. Our synthetic approach will offer guidance for developing highly active electrocatalysts utilizing multinuclear metal sites not only for the ORR but also for other electrocatalytic reactions.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Energy Materials, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Type: article (author version)
Appears in Collections:環境科学院・地球環境科学研究院 (Graduate School of Environmental Science / Faculty of Environmental Earth Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 加藤 優

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