Issue 40, 2018, Issue in Progress

Silicon-coordinated nitrogen-doped graphene as a promising metal-free catalyst for N2O reduction by CO: a theoretical study

Abstract

Metal-free catalysts for the transformation of N2O and CO into green products under mild conditions have long been expected. The present work proposes using silicon-coordinated nitrogen-doped graphene (SiN4G) as a catalyst for N2O reduction and CO oxidation based on periodic DFT calculations. The reaction proceeds via two steps, which are N2O reduction at the Si reaction center, producing Si–O*, which subsequently oxidizes CO to CO2. The N2O reduction occurs with an activation energy barrier of 0.34 eV, while the CO oxidation step requires an energy of 0.66 eV. The overall reaction is highly exothermic, with a reaction energy of −3.41 eV, mostly due to the N2 generation step. Compared to other metal-free catalysts, SiN4G shows the higher selectivity because it not only strongly prefers to adsorb N2O over CO, but the produced N2 and CO2 are easily desorbed, which prevents the poisoning of the active catalytic sites. These results demonstrate that SiN4G is a promising metal-free catalyst for N2O reduction and CO oxidation under mild conditions, as the reaction is both thermodynamically and kinetically favorable.

Graphical abstract: Silicon-coordinated nitrogen-doped graphene as a promising metal-free catalyst for N2O reduction by CO: a theoretical study

Supplementary files

Article information

Article type
Paper
Submitted
17 Apr 2018
Accepted
12 Jun 2018
First published
19 Jun 2018
This article is Open Access
Creative Commons BY license

RSC Adv., 2018,8, 22322-22330

Silicon-coordinated nitrogen-doped graphene as a promising metal-free catalyst for N2O reduction by CO: a theoretical study

A. Junkaew, S. Namuangruk, P. Maitarad and M. Ehara, RSC Adv., 2018, 8, 22322 DOI: 10.1039/C8RA03265C

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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