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

Pakrieva, Ekaterina (Universidad de Zaragoza) ; Hernandez-Ferrer, Javier ; Martinez, Gema ; Balas, Francisco (Universidad de Zaragoza) ; García-Bordeje, Enrique ; Anson-Casaos, Alejandro ; Simonelli, Laura ; Bartolome, Fernando ; Benito, Ana M. ; Maser, Wolfgang K. ; Hueso, Jose L. (Universidad de Zaragoza) ; Santamaria, Jesus (Universidad de Zaragoza)

Resumen: 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.

Idioma: Inglés

DOI: 10.1016/j.cej.2025.171198

Año: 2025

Publicado en: Chemical Engineering Journal 526 (2025), 171198 [13 pp.]
ISSN: 1385-8947

Financiación: info:eu-repo/grantAgreement/ES/AEI/CEX2023-001286-S
Financiación: info:eu-repo/grantAgreement/ES/AEI/PID2020-114926RB-I00
Financiación: info:eu-repo/grantAgreement/ES/AEI/PID2023-146481OB-I00
Financiación: info:eu-repo/grantAgreement/ES/DGA/T03-23R
Financiación: info:eu-repo/grantAgreement/ES/UZ-DGA/T57-23R
Financiación: info:eu-repo/grantAgreement/ES/MICINN/CNS2022-135911
Financiación: info:eu-repo/grantAgreement/ES/MICINN/JDC2022-049007-I
Financiación: info:eu-repo/grantAgreement/ES/MICINN/PID2022-139671OB-I00

Tipo y forma: Article (Published version)

Área (Departamento): Área Ingeniería Química (Dpto. Ing.Quím.Tecnol.Med.Amb.)
Área (Departamento): Área Tecnologi. Medio Ambiente (Dpto. Ing.Quím.Tecnol.Med.Amb.)