Issue 12, 2023

2D carbon nitride as a support with single Cu, Ag, and Au atoms for carbon dioxide reduction reaction

Abstract

The electrochemical conversion of CO2 into value-added chemicals is an important approach to recycling CO2. In this work, we have combined the most efficient metal catalysts for this reaction, namely Cu, Ag, and Au, as single-atom particles dispersed on a two-dimensional carbon nitride support, with the aim of exploring their performance in the CO2 reduction reaction. Here, we report density functional theory computations showing the effect of single metal-atom particles on the support. We found that bare carbon nitride needed a high overpotential to overcome the energy barrier for the first proton–electron transfer, while the second transfer was exergonic. The deposition of single metal atoms enhances the catalytic activity of the system as the first proton–electron transfer is favored in terms of energy, although strong binding energies were found for CO adsorption on Cu and Au single atoms. Our theoretical interpretations are consistent with the experimental evidence that the competitive H2 generation is favored due to the strong CO binding energies. Our computational study paves the road to finding suitable metals that catalyze the first proton–electron transfer in the carbon dioxide reduction reaction and produce reaction intermediates with moderate binding energies, promoting a spillover to the carbon nitride support and thereby serving as bifunctional electrocatalysts.

Graphical abstract: 2D carbon nitride as a support with single Cu, Ag, and Au atoms for carbon dioxide reduction reaction

Supplementary files

Article information

Article type
Paper
Submitted
25 Jan 2023
Accepted
21 Feb 2023
First published
23 Feb 2023
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2023,25, 8574-8582

2D carbon nitride as a support with single Cu, Ag, and Au atoms for carbon dioxide reduction reaction

S. Posada-Pérez, A. Vidal-López, M. Solà and A. Poater, Phys. Chem. Chem. Phys., 2023, 25, 8574 DOI: 10.1039/D3CP00392B

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