Regulating the frontier orbital of iron phthalocyanine with nitrogen doped carbon nanosheets for improving oxygen reduction activity

Iron phthalocyanine (FePc) has attracted widespread attention for its tunable electronic structure. However, the Fe-N sites suffer from undesirable oxygen reduction activity due to the symmetric geometries. A suitable substrate was thus needed to induce electron redistribution around Fe-N to improve...

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Bibliographic Details
Published in:Nanoscale 2024-04, Vol.16 (16), p.836-845
Main Authors: Zhang, Xilin, Zheng, Rui, Chang, Qingfang, Ma, Zhongjun, Yang, Zongxian
Format: Article
Language:English
Subjects:
Carbon
Catalysts
Electronic structure
Electrons
High temperature
Iron
Metal air batteries
Metal phthalocyanines
Nanosheets
Nitrogen
Pyrolysis
Rechargeable batteries
Substrates
Zinc-oxygen batteries
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Summary:Iron phthalocyanine (FePc) has attracted widespread attention for its tunable electronic structure. However, the Fe-N sites suffer from undesirable oxygen reduction activity due to the symmetric geometries. A suitable substrate was thus needed to induce electron redistribution around Fe-N to improve the activity. Herein, ultrathin nitrogen-doped carbon nanosheets (N-CNSs) were prepared by a simple high temperature pyrolysis. Then iron phthalocyanine was loaded on the ultrathin nitrogen-doped carbon nanosheets (FePc@N-CNSs) by a low-cost and simple solution method. This composite catalyst shows an excellent ORR activity with a half potential of 0.88 V, an onset potential of 0.99 V and durability superior to commercial Pt/C. When used as an air cathode catalyst for rechargeable zinc-air batteries, FePc@N-CNS modified batteries outperform Pt/C + RuO 2 modified batteries with higher power density and superior constant current charge-discharge cycling stability of 37 hours. The regulated electronic structure of FePc by the N-CNS substrate was revealed further by DFT calculations, which explained the enhanced adsorption of the active center to the intermediates and the increased ORR performance. N-CNSs facilitate the redistribution of electrons in FePc. The localized electrons near the Fermi level of an Fe atom play a key role in enhancing the interaction between the catalyst and intermediates, contributing to an enhanced activity.
ISSN:2040-3364
2040-3372
DOI:10.1039/d4nr00377b