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Impact of Heterometallic Cooperativity of Iron and Copper Active Sites on Electrocatalytic Oxygen Reduction Kinetics

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Title: Impact of Heterometallic Cooperativity of Iron and Copper Active Sites on Electrocatalytic Oxygen Reduction Kinetics
Authors: Kato, Masaru Browse this author →KAKEN DB
Fujibayashi, Natsuki Browse this author
Abe, Daiki Browse this author
Matsubara, Naohiro Browse this author
Yasuda, Satoshi Browse this author →KAKEN DB
Yagi, Ichizo Browse this author →KAKEN DB
Keywords: non-PGM
oxygen reduction reaction
polymer electrolyte fuel cell
oxygen reduction kinetics
bio-inspired approach
heterobimetallic active sites
Issue Date: 19-Feb-2021
Publisher: American Chemical Society(ACS)
Journal Title: ACS Catalysis
Volume: 11
Issue: 4
Start Page: 2356
End Page: 2365
Publisher DOI: 10.1021/acscatal.0c04753
Abstract: The oxygen reduction reaction (ORR) is a key reaction in polymer electrolyte fuel cells and metal–air batteries. In these electrochemical systems, platinum group metals (PGMs) have been widely used as ORR electrocatalysts. Because of material cost and scarcity of platinum group metals, non-PGM electrocatalysts are considered to be an ideal alternative for mass production with low material cost. Many non-PGM electrocatalysts have been intensively studied such as pyrolyzed Fe-, N-doped carbon (Fe–N–C) catalysts. However, many non-PGM electrocatalysts including Fe–N–C still suffer from product selectivity due to the production of H2O2 as the byproduct. In this work, we synthesized an ORR electrocatalyst of Cu-, Fe-, and N-doped carbon nanotubes, (Cu,Fe)–N–CNT. This heterobimetallic catalyst showed the selective 4e– reduction of O2 to H2O with ca. 99%. Kinetic analysis of the electrocatalytic ORR and hydrogen peroxide reduction reaction (HPRR) in acidic media revealed that (Cu,Fe)–N–CNT showed two orders of magnitude higher rate constants for the direct 4e– reduction of O2 to H2O than those for the 2e– reduction of O2 to H2O2, whereas a monometallic Fe–N–CNT showed the same order of magnitude, indicating that the heterometallic cooperativity had a drastic impact on the ORR kinetics. Our findings would open up possibilities to develop non-PGM ORR electrocatalysts with heterobimetallic active sites for the selective ORR.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, 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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