Mechanism of Low Pressure Plasma-Assisted CO2 Hydrogenation Over Ni-USY by Microsecond Time-resolved FTIR Spectroscopy

• Published in: Topics in catalysis Vol. 60; no. 19-20; pp. 1709 - 1721
• Main Authors: Azzolina-Jury, Federico, Thibault-Starzyk, Frédéric
• Format: Journal Article
• Language: English
• Published: New York Springer US 01.12.2017; Springer Nature B.V; Springer Verlag [1994-....]
• Subjects: Carbon dioxide; Carbonates; Carbonyls; Catalysis; Catalysts; Characterization and Evaluation of Materials; Chemical Sciences; Chemistry; Chemistry and Materials Science; Formates; Fourier transforms; Hydrogenation; Industrial Chemistry/Chemical Engineering; Infrared spectroscopy; Low pressure; Methane; Nickel; Original Paper; Pharmacy; Physical Chemistry; Plasma; Time-resolved FTIR; CO; hydrogenation; Zeolite USY; Mechanism; Glow discharge
• ISSN: 1022-5528; 1572-9028
• DOI: 10.1007/s11244-017-0849-2

Zeolite H-USY doped with nickel (14% wt.) was used as a catalyst in the plasma-assisted CO 2 hydrogenation under partial vacuum. CO was found to be the main product of the reaction and it is generated by plasma-assisted CO 2 dissociation in the gas phase. The CO 2 molecules vibrationally excited by plasma are also adsorbed on metallic nickel as formates which are further transformed into linear carbonyls. These species are then hydrogenated to form methane. Since the catalyst presents a low basic behavior, methane is produced from hydrogenation of linear carbonyls on nickel surface rather than from carbonates species. A detailed mechanism for this reaction assisted by plasma (glow discharge) is proposed using Operando time-resolved FTIR spectroscopic data.