Combined Experimental and Theoretical Study of Cobalt Corroles as Catalysts for Oxygen Reduction Reaction

Jennifer S. Shpilman, Ariel Friedman, Noam Zion, Naomi Levy, Dan T. Major, Lior Elbaz

Research output: Contribution to journalArticlepeer-review

23 Scopus citations

Abstract

Bioinspired transition-metal complexes may serve as efficient and low-cost potential catalysts for oxygen reduction reaction (ORR) in fuel cells, instead of precious group metal-free (PGM-free) materials. Herein, we present a study of the ORR electrocatalytic activity of different mesosubstituted Co-corroles with varying electronegativity using both experimental and theoretical methods. Specifically, we studied the influence of different mesosubstituted Co-corroles on catalytic activity. Using density functional theory (DFT), we computed lowest unoccupied molecular orbital (LUMO) energies, vertical excitation energies, electrostatic potentials, and O2 adsorption energies and compared them with the ORR catalytic activity obtained from cyclic voltammetry and rotating ring-disk electrode measurements. We found that the first one-electron reduction for all the corroles occurs at the Co-center based on computed LUMOs, and that this is a necessary step for the ORR mechanism to take place. The ORR reduction potential trends observed from theory and experiments are in good agreement. Based on this work, we conclude that the role of the substituents is significant and an important factor that affects the overpotential required for the ORR.

Original languageEnglish
Pages (from-to)30129-30136
Number of pages8
JournalJournal of Physical Chemistry C
Volume123
Issue number50
DOIs
StatePublished - 19 Dec 2019

Bibliographical note

Publisher Copyright:
© 2019 American Chemical Society.

Fingerprint

Dive into the research topics of 'Combined Experimental and Theoretical Study of Cobalt Corroles as Catalysts for Oxygen Reduction Reaction'. Together they form a unique fingerprint.

Cite this