Issue 13, 2023

Methane activation with nitric oxide at low temperatures on supported Pt catalysts: effects of the support

Abstract

Platinum nanoparticles supported on various metal oxides (MgO, (θ + γ)-Al2O3, SiO2, TiO2, Y2O3, ZrO2, and CeO2) were examined for the catalytic activation of methane with nitric oxide at low temperatures (300–400 °C) and atmospheric pressure. The catalysts exhibited similar levels of CH4 and NO conversion, except for those supported on the basic oxides (MgO and Y2O3). Notably, hydrogen cyanide (HCN), a widely used chemical intermediate, was detected in an appreciable amount only on the (θ + γ)-Al2O3-supported Pt catalyst. A more detailed comparison of the Pt nanoparticles dispersed on SiO2, TiO2, and (θ + γ)-Al2O3 indicated that the difference in the catalytic behavior for C–N coupling was not related to the electronic and geometric properties of Pt, but rather stems from the relative concentrations of adsorbed CHx and NO species. A combination of reactivity and in situ spectroscopic results suggest that a much higher surface concentration of NO relative to CHx may be responsible for the easier reduction of NO to form N2 and N2O on Pt/SiO2 and Pt/TiO2. Along the same vein, comparable concentrations of NO and CHx may be responsible for the formation of HCN on Pt/(θ + γ)-Al2O3. A further comparison of Pt catalysts supported on Al2O3 with different crystal structures (α-Al2O3, θ-Al2O3, (θ + γ)-Al2O3, and γ-Al2O3) confirmed the favorable properties of Al2O3 in HCN formation, although a preponderance of surface acidic OH groups on the supports promoted subsequent hydrolysis of HCN to NH3.

Graphical abstract: Methane activation with nitric oxide at low temperatures on supported Pt catalysts: effects of the support

Supplementary files

Article information

Article type
Paper
Submitted
22 apr 2023
Accepted
02 iyn 2023
First published
03 iyn 2023

Catal. Sci. Technol., 2023,13, 3927-3939

Author version available

Methane activation with nitric oxide at low temperatures on supported Pt catalysts: effects of the support

N. Suganuma, I. T. Ghampson, H. Miura, J. Murakami, K. K. Bando, T. Kodaira, T. Yamasaki, A. Takagaki, T. Ishihara and T. Shishido, Catal. Sci. Technol., 2023, 13, 3927 DOI: 10.1039/D3CY00555K

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