Issue 8, 2022

New insights into the key bifunctional role of sulfur in Fe–N–C single-atom catalysts for ORR/OER

Abstract

Sulfur-doping of non-noble metal Fe–N–C single-atom catalysts (SACs) shows a key bifunctional role in promoting ORR and OER activity. The controversial claims about the enhanced ORR activity and the ambiguity of the OER activity brought about by S-doping demand in-depth investigation. Here, systematic theoretical investigation was carried out. Unlike previously believed, coordinative S-doping gives rise to a precisely regulated OOH* stabilization effect, which is revealed to be the origin of the bifunctional ORR/OER activity. The fine regulation is reflected in two aspects: (1) Compared with other intermediates, the regulation of OOH* adsorption is more obvious. (2) More sulfur-doping leads to excessive strong or weak stabilization, which is not conducive to ORR/OER. The single S doping elevates the charge density and opens the metallic spin channels of Fe–N3|S, moves the d-band center towards the Fermi level, all contributing to moderate OOH* stabilization. It is hoped that these results will promote the development of heteroatom-doped bifunctional SACs.

Graphical abstract: New insights into the key bifunctional role of sulfur in Fe–N–C single-atom catalysts for ORR/OER

Supplementary files

Article information

Article type
Paper
Submitted
29 Huk 2021
Accepted
26 Sun 2022
First published
27 Sun 2022

Nanoscale, 2022,14, 3212-3223

New insights into the key bifunctional role of sulfur in Fe–N–C single-atom catalysts for ORR/OER

X. Zhang, Q. Zhang, J. Cui, J. Yan, J. Liu and Y. Wu, Nanoscale, 2022, 14, 3212 DOI: 10.1039/D1NR07851H

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