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One-Step Preparation of Fe/N/C Single-Atom Catalysts Containing Fe-N-4 Sites from an Iron Complex Precursor with 5,6,7,8-Tetraphenyl-1,12-Diazatriphenylene Ligands

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Please use this identifier to cite or link to this item:http://hdl.handle.net/2115/88153

Title: One-Step Preparation of Fe/N/C Single-Atom Catalysts Containing Fe-N-4 Sites from an Iron Complex Precursor with 5,6,7,8-Tetraphenyl-1,12-Diazatriphenylene Ligands
Authors: Matsumoto, Koki Browse this author
Kato, Masaru Browse this author →KAKEN DB
Yagi, Ichizo Browse this author →KAKEN DB
Xie, Siqi Browse this author
Asakura, Kiyotaka Browse this author →KAKEN DB
Noro, Shin-Ichiro Browse this author →KAKEN DB
Tohnai, Norimitsu Browse this author →KAKEN DB
Campidelli, Stephane Browse this author
Hayashi, Takashi Browse this author →KAKEN DB
Onoda, Akira Browse this author →KAKEN DB
Keywords: Fe/N/C single-atom catalysts
Fe-N-4 sites
iron-diazatriphenylene complexes
one-step preparation
oxygen reduction reaction (ORR)
Issue Date: 24-Jan-2022
Publisher: Wiley-Blackwell
Journal Title: Chemistry-A European Journal
Volume: 28
Issue: 5
Start Page: e202103545
Publisher DOI: 10.1002/chem.202103545
Abstract: Fe/N/C single-atom catalysts containing Fe-N-x sites prepared by pyrolysis are promising cathode materials for fuel cells and metal-air batteries due to their high oxygen reduction reaction (ORR) activities. We have developed iron complexes containing N2- or N3-chelating coordination structures with preorganized aromatic rings in a 1,12-diazatriphenylene framework tethering bromo substituents as precursors to precisely construct Fe-N-4 sites in an Fe/N/C catalyst. One-step pyrolysis of the iron complex with carbon black forms atomically dispersed Fe-N-4 sites without iron aggregates. X-ray absorption spectroscopy (XAS) and electrochemical measurements revealed that the iron complex with N3-coordination is more effectively converted to Fe-N-4 sites catalyzing ORR with a TOF value of 0.21 e site(-1) s(-1) at 0.8V vs. RHE. This indicates that the formation of Fe-N-4 sites is controlled by precise tuning of the chemical structure of the iron complex precursor.
Rights: This is the peer reviewed version of the following article: K. Matsumoto, M. Kato, I. Yagi, S. Xie, K. Asakura, S.-i. Noro, N. Tohnai, S. Campidelli, T. Hayashi, A. Onoda, Chem. Eur. J. 2022, 28(5), e202103545, which has been published in final form at https://doi.org/10.1002/chem.202103545. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
Type: article (author version)
URI: http://hdl.handle.net/2115/88153
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: 小野田 晃

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