Jump to main content
Jump to site search

Issue 27, 2014
Previous Article Next Article

A density functional theory study of oxygen reduction reaction on non-PGM Fe–Nx–C electrocatalysts

Author affiliations

Abstract

First-principles density functional theory (DFT) calculations were performed to explain the stability of catalytically active sites in Fe–Nx–C electrocatalysts, their ORR activity and ORR mechanism. The results show that the formation of graphitic in-plane Fe–N4 sites in a carbon matrix is energetically favorable over the formation of Fe–N2 sites. Chemisorption of ORR species O2, O, OH, OOH, and H2O and O–O bond breaking in peroxide occur on both Fe–N2 and Fe–N4 sites. In addition to the favorable interaction of ORR species, the computed free energy diagrams show that elementary ORR reaction steps on Fe–Nx sites are downhill. Thus, a complete ORR is predicted to occur via a single site 4e mechanism on graphitic Fe–Nx (x = 2, 4) sites. Because of their higher stability and working potential for ORR, Fe–N4 sites are predicted to be prime candidate sites for ORR in pyrolyzed Fe–Nx–C electrocatalysts.

Graphical abstract: A density functional theory study of oxygen reduction reaction on non-PGM Fe–Nx–C electrocatalysts

Back to tab navigation

Supplementary files

Article information


Submitted
16 Apr 2014
Accepted
15 May 2014
First published
15 May 2014

Phys. Chem. Chem. Phys., 2014,16, 13800-13806
Article type
Paper

A density functional theory study of oxygen reduction reaction on non-PGM Fe–Nx–C electrocatalysts

S. Kattel, P. Atanassov and B. Kiefer, Phys. Chem. Chem. Phys., 2014, 16, 13800
DOI: 10.1039/C4CP01634C

Social activity

Search articles by author

Spotlight

Advertisements