Engineering single-atom Fe-N active sites on hollow carbon spheres for oxygen reduction reaction

• Type: Article in International Scientific Journal
• Date: 2023

Authors

Rui S. Ribeiro (Author) FEUP; Ana L.S. Viera (Author) Other; Krzysztof Biernacki (Author) FEUP; Alexandre L. Magalhães (Author) FCUP; Juan J. Delgado (Author) Other; Rafael G. Morais (Author) Other; Natalia Rey-Raap (Author) Other; Raquel P. Rocha (Author) FEUP; M. Fernando R. Pereira (Author) FEUP

Journal

Title: Carbon

Vol. 213 No. 118192

ISSN: 0008-6223

Publisher: Elsevier

Indexing

ISI Web of Knowledge - 1 Citation

Scopus

Associated Projects

BiCat4Energy - Electrocatalisadores bifuncionais baseados em materiais de carbono isentos de metais nobres para a produção de energia renovável: melhoramento da tecnologia da Célula de Combustível Unitária Regenerativa.

HyGreen&LowEmissions - HyGreen&LowEmissions - Tackling Climate Change Impacts: the role of Green Hydrogen production, storage and use, together with low emissions energy systems

LA LSRE-LCM - Financiamento Plurianual 2020-2023 para a Unidade LA LSRE-LCM Laboratório de Processos de Separação e Reacção - Laboratório de Catálise e Materiais

Other information

Authenticus ID: P-00Y-HGT

DOI: 10.1016/j.carbon.2023.118192

Abstract (EN): Seeking alternatives to noble metals-based electrocatalysts for oxygen reduction reaction (ORR), hollow carbon spheres (CSs) were finely tuned with stable single-atom Fe-N species through a synthesis methodology requiring only earth-abundant metal precursors. CSs with different sizes were synthesized by sol-gel polycondensation of resorcinol with formaldehyde over silica nanoparticles, followed by thermal annealing and silica etching. A catalyst screening revealed the positive impact of both the hollow core and structural defects of the CSs for ORR. Single-atom Fe-N active sites were introduced on the best performing CSs through simultaneous incorporation of iron and nitrogen precursors, and glucose. A significant enhancement in ORR activity was observed despite the small iron load introduced (0.12 wt%). ORR performance indicators, advanced characterization, and molecular simulation studies revealed nitrogen's crucial role in anchoring individual iron atoms and modulating the charge density nearby the active sites (increase of 80 mV in the half-wave potential). Adding glucose as a chelating agent enhances the metal-heteroatom coordination and subsequent dispersion of iron, accounting for an increase of 20 mV in the half-wave potential, an average of electrons transferred as high as 3.9 (at 0.4 V vs. RHE), and higher stability (99%) than that of a platinum-based (20 wt%) electrocatalyst (92%).

Language: English

Type (Professor's evaluation): Scientific

No. of pages: 11