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

Kato, Masaru; Fujibayashi, Natsuki; Abe, Daiki; Matsubara, Naohiro; Yasuda, Satoshi; Yagi, Ichizo

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

Kato, Masaru; Fujibayashi, Natsuki; Abe, Daiki et al.

ACS Catalysis, 2021, 11(4), 2356-2365

Permalink : https://hdl.handle.net/2115/84178

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アクセス権	open access
URI	https://hdl.handle.net/2115/84178
タイトル	Impact of Heterometallic Cooperativity of Iron and Copper Active Sites on Electrocatalytic Oxygen Reduction Kinetics
著者	Kato, Masaru ; Fujibayashi, Natsuki ; Abe, Daiki ; Matsubara, Naohiro ; Yasuda, Satoshi ; Yagi, Ichizo
e-Rad_Researcher 70709633 著者名 Kato, Masaru
著者名 Fujibayashi, Natsuki
著者名 Abe, Daiki
著者名 Matsubara, Naohiro
e-Rad_Researcher 90400639 著者名 Yasuda, Satoshi
e-Rad_Researcher 40292776 著者名 Yagi, Ichizo
言語	英語
キーワード	non-PGM
	oxygen reduction reaction
	electrocatalysis
	polymer electrolyte fuel cell
	oxygen reduction kinetics
	bio-inspired approach
	heterobimetallic active sites
発行日	2021-02-19
出版者	American Chemical Society(ACS)
収録物名	ACS Catalysis
巻(号)	11(4)
ページ	2356-2365
抄録	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.
資源タイプ	学術雑誌論文
出版タイプ	Accepted Manuscript
権利情報	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 https://doi.org/10.1021/acscatal.0c04753
PISSN	2155-5435
NCID	AA12599706
関連情報 (isVersionOf)	出版社版DOI https://doi.org/10.1021/acscatal.0c04753