Issue 24, 2024

Catalytic oxidation mechanism of ethyl acetate on O-ligand-single-atom-Ni/2-dimensional reduced graphene oxide: the essential role of the O ligand

Abstract

Ligands play an important role in the dispersion of metal and catalytic activity in single-atom transition metal-doped catalysts (SATMCs). In this work, a series of oxygen-ligand (O-ligand)-single-atom-Ni/2-dimensional reduced graphene oxide (RGO) materials (SANiX-O-2DRGO (X = 0.5–5)) were fabricated by a simple one-step co-reduction method. The single Ni atom on SANi5-O-2DRGO is embedded into the RGO and ligated by four O-ligand atoms. A systematic study confirms that the O-ligand is conducive to the dispersion of Ni and the formation of SATMCs with high metal loading. Density functional theory (DFT) calculation results demonstrate that the d-band center value of O-ligand-single-atom-Ni is closer to the Fermi level than that of the conventional N coordination, which is beneficial for electronic transition and enhances catalytic activity, i.e., the O-ligand accelerates the electron transfer between the carrier and the single metal atom, thus improving the catalytic oxidation capacity of volatile organic compounds (VOCs) on SANi5-O-2DRGO. As a demonstration, SANi5-O-2DRGO exhibits excellent reusability, water resistance, and stability for ethyl acetate oxidation. The degradation of ethyl acetate remained at 100% over 150 hours of continuous onstream operation. The catalytic oxidation mechanism of ethyl acetate on SANi5-O-2DRGO was also investigated. The O-ligand atoms provide the key electron transfer in the activation of adsorbed oxygen and catalytic oxidation process of reaction intermediates.

Graphical abstract: Catalytic oxidation mechanism of ethyl acetate on O-ligand-single-atom-Ni/2-dimensional reduced graphene oxide: the essential role of the O ligand

Supplementary files

Article information

Article type
Paper
Submitted
16 Feb 2024
Accepted
08 May 2024
First published
08 May 2024

J. Mater. Chem. A, 2024,12, 14698-14708

Catalytic oxidation mechanism of ethyl acetate on O-ligand-single-atom-Ni/2-dimensional reduced graphene oxide: the essential role of the O ligand

X. Wang, J. Li, J. Li, B. Jing, Y. Sun, T. Wang, D. Li, H. Huang and Z. Ao, J. Mater. Chem. A, 2024, 12, 14698 DOI: 10.1039/D4TA01073F

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