Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework

Single Fe atoms dispersed on hierarchically structured porous carbon (SA‐Fe‐HPC) frameworks are prepared by pyrolysis of unsubstituted phthalocyanine/iron phthalocyanine complexes confined within micropores of the porous carbon support. The single‐atom Fe catalysts have a well‐defined atomic dispers...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2018-07, Vol.57 (29), p.9038-9043
Main Authors: Zhang, Zhengping, Sun, Junting, Wang, Feng, Dai, Liming
Format: Article
Language:English
Subjects:
Atomic structure
Carbon
Catalysis
Catalysts
Chemical reduction
Coordination compounds
Dispersion
electrocatalysis
Electrochemistry
Electrodes
Fuels
hierarchical porous carbon
Iron
Metal phthalocyanines
Oxygen
oxygen reduction reaction (ORR)
Oxygen reduction reactions
Platinum
Pneumatics
Pyrolysis
Selectivity
single-atom catalysts
Stability
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Summary:Single Fe atoms dispersed on hierarchically structured porous carbon (SA‐Fe‐HPC) frameworks are prepared by pyrolysis of unsubstituted phthalocyanine/iron phthalocyanine complexes confined within micropores of the porous carbon support. The single‐atom Fe catalysts have a well‐defined atomic dispersion of Fe atoms coordinated by N ligands on the 3D hierarchically porous carbon support. These SA‐Fe‐HPC catalysts are comparable to the commercial Pt/C electrode even in acidic electrolytes for oxygen reduction reaction (ORR) in terms of the ORR activity (E1/2=0.81 V), but have better long‐term electrochemical stability (7 mV negative shift after 3000 potential cycles) and fuel selectivity. In alkaline media, the SA‐Fe‐HPC catalysts outperform the commercial Pt/C electrode in ORR activity (E1/2=0.89 V), fuel selectivity, and long‐term stability (1 mV negative shift after 3000 potential cycles). Thus, these nSA‐Fe‐HPCs are promising non‐platinum‐group metal ORR catalysts for fuel‐cell technologies. Stay single: Single‐atom catalysts with Fe atoms dispersed on hierarchical porous carbons were prepared by pyrolysis of iron phthalocyanine and unsubstituted phthalocyanine complexes confined within micropores of the porous carbon supports. The resulting catalysts outperformed the commercial Pt/C electrode in alkaline electrolytes and showed an electrocatalytic activity comparable to the commercial Pt/C electrode in acidic media with a better long‐term stability.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201804958