Electronically and Geometrically Modified Single‐Atom Fe Sites by Adjacent Fe Nanoparticles for Enhanced Oxygen Reduction

Fe–N–C materials exhibit excellent activity and stability for oxygen reduction reaction (ORR), as one of the most promising candidates to replace commercial Pt/C catalysts. However, it is challenging to unravel features of the superior ORR activity originating from Fe–N–C materials. In this work, th...

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Vydáno v:Advanced materials (Weinheim) Ročník 34; číslo 5; s. e2107291 - n/a
Hlavní autoři: Zhao, Shu‐Na, Li, Jun‐Kang, Wang, Rui, Cai, Jinmeng, Zang, Shuang‐Quan
Médium: Journal Article
Jazyk:angličtina
Vydáno: Germany Wiley Subscription Services, Inc 01.02.2022
Témata:
atomic Fe N(O) x sites
electronic modification
Electronic structure
Fe nanoparticles
geometric modification
Iron
Materials science
Nanoparticles
oxygen reduction reaction
Oxygen reduction reactions
Single atom catalysts
Strong interactions (field theory)
electronic modification
atomic Fe N(O) x sites
geometric modification
oxygen reduction reaction
Fe nanoparticles
ISSN:0935-9648, 1521-4095, 1521-4095
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Shrnutí:Fe–N–C materials exhibit excellent activity and stability for oxygen reduction reaction (ORR), as one of the most promising candidates to replace commercial Pt/C catalysts. However, it is challenging to unravel features of the superior ORR activity originating from Fe–N–C materials. In this work, the electronic and geometric structures of the isolated Fe–N–C sites and their correlations with the ORR performance are investigated by varying the secondary thermal activation temperature of a rationally designed NC‐supported Fe single‐atom catalyst (SAC). The systematic analyses demonstrate the significant role of coordinated atoms of SA and metallic Fe nanoparticles (NPs) in altering the electronic structure of isolated Fe–N–C sites. Meanwhile, strong interaction between isolated Fe–N–C sites and adjacent Fe NPs can change the geometric structure of isolated Fe–N–C sites. Theoretical calculations reveal that optimal regulation of the electronic and geometric structure of isolated Fe–N–C sites by the co‐existence of Fe NPs narrows the energy barriers of the rate‐limiting steps of ORR, resulting in outstanding ORR performance. This work not only provides the fundamental understanding of the underlying structure–activity relationship, but also sheds light on designing efficient Fe–N–C catalysts. The correlations between electronic and geometric structures of isolated Fe–N–C sites and their oxygen reduction reaction (ORR) performance are investigated by varying the secondary heat‐treatment of a NC‐supported Fe single‐atom catalyst. The adjacent Fe nanoparticles can regulate the electronic and geometric structure of isolated Fe–N–C sites, reducing energy barriers of the rate‐limiting steps of ORR, resulting in outstanding ORR performance.
Bibliografie:ObjectType-Article-1
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ISSN:0935-9648
1521-4095
1521-4095
DOI:10.1002/adma.202107291