3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors

The sluggish kinetics of the oxygen reduction reaction (ORR) remain a key bottleneck for the commercialization of proton exchange membrane fuel cells (PEMFCs), driving the search for efficient, non-precious metal catalysts. Herein, we present a laser-assisted pyrolysis strategy for the synthesis of...

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Autores: Pakrieva, Ekaterina, Hernandez-Ferrer, Javier, Martinez, Gema, Balas, Francisco, García-Bordeje, Enrique, Anson-Casaos, Alejandro, Simonelli, Laura, Bartolome, Fernando, Benito, Ana M., Maser, Wolfgang K., Hueso, Jose L., Santamaria, Jesus
Tipo de documento: artigo
Estado:Versão publicada
Data de publicação:2025
País:España
Recursos:Universidad de Zaragoza
Repositório:Zaguán. Repositorio Digital de la Universidad de Zaragoza
OAI Identifier:oai:zaguan.unizar.es:165227
Acesso em linha:http://zaguan.unizar.es/record/165227
Access Level:Acceso aberto
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spelling 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursorsPakrieva, EkaterinaHernandez-Ferrer, JavierMartinez, GemaBalas, FranciscoGarcía-Bordeje, EnriqueAnson-Casaos, AlejandroSimonelli, LauraBartolome, FernandoBenito, Ana M.Maser, Wolfgang K.Hueso, Jose L.Santamaria, JesusThe sluggish kinetics of the oxygen reduction reaction (ORR) remain a key bottleneck for the commercialization of proton exchange membrane fuel cells (PEMFCs), driving the search for efficient, non-precious metal catalysts. Herein, we present a laser-assisted pyrolysis strategy for the synthesis of nitrogen-doped carbon (NC) materials, both metal-free and containing atomically dispersed Fe and Co, using aerosolized phthalocyanine precursors and a near-instantaneous rapid decomposition under a high-energy laser beam, while preventing metal aggregation. A single-step post-synthetic thermal activation under an NH₃/N₂ atmosphere further tailors the textural and surface properties, without requiring ammonia co-feeding during laser pyrolysis, acid etching, or multiple treatments, marking a significant improvement over our previously reported single atom (Fe-N/C) protocols. The resulting Fe_Co/NC_tr catalyst exhibits high specific surface area, enhanced microporosity, improved graphitization, and increased abundance of electrochemically beneficial nitrogen sites. Compared to our earlier reported Fe–N/C catalysts, Fe_Co/NC_tr delivers significantly higher limiting current densities and enhanced durability in alkaline media. Overall, the developed Fe_Co/NC catalyst exhibits good ORR catalytic activity and outstanding long-term stability in alkaline media, comparable to the state-of-the-art commercial Pt/C catalysts. Cyanide poisoning tests confirm the essential role of atomically dispersed Fe2+ and Co2+ as active ORR sites.2025info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://zaguan.unizar.es/record/165227reponame:Zaguán. Repositorio Digital de la Universidad de Zaragozainstname:Universidad de ZaragozaInglésinfo:eu-repo/grantAgreement/ES/AEI/CEX2023-001286-Sinfo:eu-repo/grantAgreement/ES/AEI/PID2020-114926RB-I00info:eu-repo/grantAgreement/ES/AEI/PID2023-146481OB-I00info:eu-repo/grantAgreement/ES/DGA/T03-23Rinfo:eu-repo/grantAgreement/ES/UZ-DGA/T57-23Rinfo:eu-repo/grantAgreement/ES/MICINN/CNS2022-135911info:eu-repo/grantAgreement/ES/MICINN/JDC2022-049007-Iinfo:eu-repo/grantAgreement/ES/MICINN/PID2022-139671OB-I00info:eu-repo/semantics/openAccessoai:zaguan.unizar.es:1652272026-05-29T13:59:51Z
dc.title.none.fl_str_mv 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
title 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
spellingShingle 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
Pakrieva, Ekaterina
title_short 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
title_full 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
title_fullStr 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
title_full_unstemmed 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
title_sort 3-component (N, Fe, Co) atomically dispersed ORR catalysts prepared by laser-driven decomposition of organic precursors
dc.creator.none.fl_str_mv Pakrieva, Ekaterina
Hernandez-Ferrer, Javier
Martinez, Gema
Balas, Francisco
García-Bordeje, Enrique
Anson-Casaos, Alejandro
Simonelli, Laura
Bartolome, Fernando
Benito, Ana M.
Maser, Wolfgang K.
Hueso, Jose L.
Santamaria, Jesus
author Pakrieva, Ekaterina
author_facet Pakrieva, Ekaterina
Hernandez-Ferrer, Javier
Martinez, Gema
Balas, Francisco
García-Bordeje, Enrique
Anson-Casaos, Alejandro
Simonelli, Laura
Bartolome, Fernando
Benito, Ana M.
Maser, Wolfgang K.
Hueso, Jose L.
Santamaria, Jesus
author_role author
author2 Hernandez-Ferrer, Javier
Martinez, Gema
Balas, Francisco
García-Bordeje, Enrique
Anson-Casaos, Alejandro
Simonelli, Laura
Bartolome, Fernando
Benito, Ana M.
Maser, Wolfgang K.
Hueso, Jose L.
Santamaria, Jesus
author2_role author
author
author
author
author
author
author
author
author
author
author
description The sluggish kinetics of the oxygen reduction reaction (ORR) remain a key bottleneck for the commercialization of proton exchange membrane fuel cells (PEMFCs), driving the search for efficient, non-precious metal catalysts. Herein, we present a laser-assisted pyrolysis strategy for the synthesis of nitrogen-doped carbon (NC) materials, both metal-free and containing atomically dispersed Fe and Co, using aerosolized phthalocyanine precursors and a near-instantaneous rapid decomposition under a high-energy laser beam, while preventing metal aggregation. A single-step post-synthetic thermal activation under an NH₃/N₂ atmosphere further tailors the textural and surface properties, without requiring ammonia co-feeding during laser pyrolysis, acid etching, or multiple treatments, marking a significant improvement over our previously reported single atom (Fe-N/C) protocols. The resulting Fe_Co/NC_tr catalyst exhibits high specific surface area, enhanced microporosity, improved graphitization, and increased abundance of electrochemically beneficial nitrogen sites. Compared to our earlier reported Fe–N/C catalysts, Fe_Co/NC_tr delivers significantly higher limiting current densities and enhanced durability in alkaline media. Overall, the developed Fe_Co/NC catalyst exhibits good ORR catalytic activity and outstanding long-term stability in alkaline media, comparable to the state-of-the-art commercial Pt/C catalysts. Cyanide poisoning tests confirm the essential role of atomically dispersed Fe2+ and Co2+ as active ORR sites.
publishDate 2025
dc.date.none.fl_str_mv 2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://zaguan.unizar.es/record/165227
url http://zaguan.unizar.es/record/165227
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/ES/AEI/CEX2023-001286-S
info:eu-repo/grantAgreement/ES/AEI/PID2020-114926RB-I00
info:eu-repo/grantAgreement/ES/AEI/PID2023-146481OB-I00
info:eu-repo/grantAgreement/ES/DGA/T03-23R
info:eu-repo/grantAgreement/ES/UZ-DGA/T57-23R
info:eu-repo/grantAgreement/ES/MICINN/CNS2022-135911
info:eu-repo/grantAgreement/ES/MICINN/JDC2022-049007-I
info:eu-repo/grantAgreement/ES/MICINN/PID2022-139671OB-I00
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv
publisher.none.fl_str_mv
dc.source.none.fl_str_mv reponame:Zaguán. Repositorio Digital de la Universidad de Zaragoza
instname:Universidad de Zaragoza
instname_str Universidad de Zaragoza
reponame_str Zaguán. Repositorio Digital de la Universidad de Zaragoza
collection Zaguán. Repositorio Digital de la Universidad de Zaragoza
repository.name.fl_str_mv
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