Issue 20, 2024

Multi-atomic loaded C2N1 catalysts for CO2 reduction to CO or formic acid

Abstract

In recent years, the development of highly active and selective electrocatalysts for the electrochemical reduction of CO2 to produce CO and formic acid has aroused great interest, and can reduce environmental pollution and greenhouse gas emissions. Due to the high utilization of atoms, atom-dispersed catalysts are widely used in CO2 reduction reactions (CO2RRs). Compared with single-atom catalysts (SACs), multi-atom catalysts have more flexible active sites, unique electronic structures and synergistic interatomic interactions, which have great potential in improving the catalytic performance. In this study, we established a single-layer nitrogen–graphene-supported transition metal catalyst (TM-C2N1) based on density functional theory, facilitating the reduction of CO2 to CO or HCOOH with single-atom and multi-atomic catalysts. For the first time, the TM-C2N1 monolayer was systematically screened for its catalytic activity with ab initio molecular dynamics, density of states, and charge density, confirming the stability of the TM-C2N1 catalyst structure. Furthermore, the Gibbs free energy and electronic structure analysis of 3TM-C2N1 revealed excellent catalytic performance for CO and HCOOH in the CO2RR with a lower limiting potential. Importantly, this work highlights the moderate adsorption energy of the intermediate on 3TM-C2N1. It is particularly noteworthy that 3Mo-C2N1 exhibited the best catalytic performance for CO, with a limiting potential (UL) of −0.62 V, while 3Ti-C2N1 showed the best performance for HCOOH, with a corresponding UL of −0.18 V. Additionally, 3TM-C2N1 significantly inhibited competitive hydrogen evolution reactions. We emphasize the crucial role of the d-band center in determining products, as well as the activity and selectivity of triple-atom catalysts in the CO2RR. This theoretical research not only advances our understanding of multi-atomic catalysts, but also offers new avenues for promoting sustainable CO2 conversion.

Graphical abstract: Multi-atomic loaded C2N1 catalysts for CO2 reduction to CO or formic acid

Supplementary files

Article information

Article type
Paper
Submitted
03 رمضان 1445
Accepted
10 شوال 1445
First published
10 شوال 1445

Nanoscale, 2024,16, 9791-9801

Multi-atomic loaded C2N1 catalysts for CO2 reduction to CO or formic acid

Y. Sun, L. Tao, M. Wu, D. Dastan, J. Rehman, L. Li and B. An, Nanoscale, 2024, 16, 9791 DOI: 10.1039/D4NR01082E

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