Affiliations 

  • 1 Research Center for Quantum Physics, National Research and Innovation Agency (BRIN), South Tangerang 15314, Indonesia. sasfan.arman.wella@brin.go.id
  • 2 Advanced Functional Materials Research Group, Faculty of Industrial Technology, Institut Teknologi Bandung, Bandung 40132, Indonesia. gandaryus@itb.ac.id
  • 3 Theoretical High Energy Physics Research Division, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Bandung 40132, Indonesia
  • 4 Mechanical Engineering Study Program, Institut Teknologi Sumatera (ITERA), South Lampung 35365, Indonesia
  • 5 Department of Chemical Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, Bangi 43600, Malaysia
Phys Chem Chem Phys, 2023 Dec 06;25(47):32637-32647.
PMID: 38009535 DOI: 10.1039/d3cp03642a

Abstract

Pyrolyzed Fe-N-C-based catalysts, particularly FeN4, are reported to show enhanced catalytic activity for some chemical reactions, particularly for the oxygen reduction reaction (ORR). Here, we present a computational study to investigate another pyrolyzed Fe-N-C-based catalyst, i.e. Fe2N6, adsorbed on graphene with special emphasis on the edges of graphene nanoribbons (both zig-zag and armchair configurations) as a candidate for Fe dual-atom catalysts (Fe-DACs). Utilizing density functional theory calculations along with microkinetic simulations, we investigate the influence of graphitic edges on the stability and ORR activity of Fe-DAC active sites. Our findings indicate that the presence of graphitic edges, particularly the zig-zag configuration, significantly lowers the formation energy of Fe-DAC active sites, making them more likely to form at the edges. Furthermore, several Fe-DAC active sites at graphitic edges exhibit exceptional ORR performance, surpassing the commonly employed FeN4 active site in SAC systems and even exceeding the benchmark Pt(111) surface. Notably, the (Fe2N6)o@z1 active site demonstrates outstanding performance in both associative and dissociative mechanisms. These results highlight the role of graphitic nanopores in enhancing the catalytic behavior of Fe-DAC active sites, providing valuable insights for designing efficient non-precious metal catalysts for ORR applications.

* Title and MeSH Headings from MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine.