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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
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)
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Submitter: 小野田 晃
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