Understanding the Deactivation of an Fe Single-Atom on Nitrogen-Doped Carbon Catalysts in Oxygen Reduction Reaction

Single-atom catalysts (SACs) have gained attention as potential replacements for the platinum-group metals (PGMs) in the oxygen reduction reaction (ORR), a fundamental reaction in renewable energy technologies. Among SACs, the Fe single-atom nitrogen-doped carbon catalysts (Fe–NxCy) are prominent du...

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Bibliographic Details
Authors: Minotaki, Maria G., López, Núria
Format: article
Publication Date:2025
Country:España
Institution:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repository:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/484677
Online Access:http://hdl.handle.net/2072/484677
https://doi.org/10.1021/acs.jpcc.5c01611
Access Level:Embargoed access
Keyword:Química
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Summary:Single-atom catalysts (SACs) have gained attention as potential replacements for the platinum-group metals (PGMs) in the oxygen reduction reaction (ORR), a fundamental reaction in renewable energy technologies. Among SACs, the Fe single-atom nitrogen-doped carbon catalysts (Fe–NxCy) are prominent due to their remarkable activity. However, their long-term stability under operando conditions remains a critical challenge. Here, we show that a carbon atom coordinated to the Fe center can activate and interact with reactive oxygen species, leading to the formation of a stabilized C–O bond. Demetallization is promoted by electronic and structural changes in the catalyst, driven by its spin-polarization state. These findings provide mechanistic insights into the deactivation of Fe–NxCy moieties and guide the design of robust and sustainable catalysts for energy applications.