One‐step Preparation of Fe/N/C Single‐atom Catalysts Containing Fe−N4 Sites from an Iron Complex Precursor with 5,6,7,8‐Tetraphenyl‐1,12‐diazatriphenylene Ligands - CEA - Commissariat à l’énergie atomique et aux énergies alternatives Accéder directement au contenu
Article Dans Une Revue Chemistry - A European Journal Année : 2022

One‐step Preparation of Fe/N/C Single‐atom Catalysts Containing Fe−N4 Sites from an Iron Complex Precursor with 5,6,7,8‐Tetraphenyl‐1,12‐diazatriphenylene Ligands

Résumé

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 0.8 V 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.

Domaines

Matériaux

Dates et versions

cea-03466860 , version 1 (06-12-2021)

Identifiants

Citer

Koki Matsumoto, Masaru Kato, Ichizo Yagi, Siqi Xie, Kiyotaka Asakura, et al.. One‐step Preparation of Fe/N/C Single‐atom Catalysts Containing Fe−N4 Sites from an Iron Complex Precursor with 5,6,7,8‐Tetraphenyl‐1,12‐diazatriphenylene Ligands. Chemistry - A European Journal, 2022, 28 (5), pp.e202103545. ⟨10.1002/chem.202103545⟩. ⟨cea-03466860⟩
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