Issue 36, 2020

Theoretical investigation on catalytic mechanisms of oxygen reduction and carbon monoxide oxidation on the MnNx system

Abstract

Single-atom catalysts (SACs) have been extensively studied due to their highly dispersed atomic levels, which greatly improve the distribution of active sites and maximum utilization of the catalyst. In this study, Mn-based SACs were modeled on N-doped graphene with single and double vacancy defects, and 11 types of MnNx models containing various three- and four-coordinate structures were considered. The ORR overpotential of MnN3 (MnN4) was lowest in the three-coordinate structure (four-coordinate structure), which was selected to study catalytic activities for the oxygen reduction reaction (ORR) and reaction mechanism. The best reaction path for ORR on MnN4 is *O2 → *O + H2O → *OH → H2O and the energy barrier of the rate-determining step (RDS) is 0.172 eV. According to the adsorption energy competition, the best catalytic performance of MnN4 was selected to study the various reaction mechanisms of carbon monoxide oxidation (COOR). The best reaction path is the CO oxidation on MnN4 along the termolecular Eley–Rideal (TER) with a RDS energy barrier of 0.218 eV. These results suggest that MnN4 is a promising bifunctional catalyst.

Graphical abstract: Theoretical investigation on catalytic mechanisms of oxygen reduction and carbon monoxide oxidation on the MnNx system

Supplementary files

Article information

Article type
Paper
Submitted
26 Jul 2020
Accepted
24 Aug 2020
First published
24 Aug 2020

New J. Chem., 2020,44, 15724-15732

Theoretical investigation on catalytic mechanisms of oxygen reduction and carbon monoxide oxidation on the MnNx system

M. Luo, Z. Liang, M. Chen, C. Liu, X. Qi, S. G. Peera, J. Liu and T. Liang, New J. Chem., 2020, 44, 15724 DOI: 10.1039/D0NJ03756G

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements