Issue 30, 2023

Rare-earth metal-N6 centers in porous carbon for electrocatalytic CO2 reduction

Abstract

Single-atom catalysts fabricated using rare earth elements have emerged for electrocatalytic carbon dioxide reduction, but they need to be studied systematically and intensively. Herein, density functional theory was employed to determine the electrocatalytic CO2 reduction activity of rare earth-N6 porous carbon (Re = Ce, Nd, Sm, Eu, Gd, Tb, Er, Tm, Yb, and Lu) single-atom catalysts. The results revealed that the binding energy of the rare-earth atoms to the N6C monolayers in the ten studied Re-N6C monatomic catalysts is much more negative than the cohesion energy of the bulk rare-earth metal, which makes rare-earth atoms stably dispersed in the N6C skeleton. CO is the primary chemical product of electrocatalytic CO2 reduction by Ce, Eu, and Lu. The primary product of the six monatomic species, i.e., Nd, Sm, Tb, Er, Tm, and Yb, is HCOOH. The dominant product of Gd is CH4. The limiting potentials of these catalysts are in the range of 0.31–0.786 V and their overpotentials are in the range of 0.06–0.707 V, all of which are relatively low, showing that they are potential and promising electrocatalysts for CO2 reduction. Subsequently, Eu-N6C was experimentally synthesized and used for electrocatalytic CO2 reduction to obtain CO products, and the overpotential showed good agreement with the theoretically calculated values.

Graphical abstract: Rare-earth metal-N6 centers in porous carbon for electrocatalytic CO2 reduction

Supplementary files

Article information

Article type
Paper
Submitted
22 May 2023
Accepted
26 Jun 2023
First published
10 Jul 2023

Phys. Chem. Chem. Phys., 2023,25, 20381-20394

Rare-earth metal-N6 centers in porous carbon for electrocatalytic CO2 reduction

X. Zeng, L. Liao, M. Wang and H. Wang, Phys. Chem. Chem. Phys., 2023, 25, 20381 DOI: 10.1039/D3CP02314A

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