Activation and Conversion of Methane to Syngas over ZrO2/Cu(111) Catalysts near Room Temperature

• Published in: Journal of the American Chemical Society Vol. 145; no. 15; pp. 8326 - 8331
• Main Authors: Huang, Erwei, Rui, Ning, Rosales, Rina, Liu, Ping, Rodriguez, José A.
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 05.04.2023; American Chemical Society (ACS)
• Subjects: 03 NATURAL GAS; catalysts; chemical reactions; copper; hydrocarbons; hydrogen; interfaces; methane; molecules; zirconium oxide
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.3c01980

Enzymatic systems achieve the catalytic conversion of methane at room temperature under mild conditions. In this study, varying thermodynamic and kinetic parameters, we show that the reforming of methane by water (MWR, CH4 + H2O → CO + 3H2) and the water–gas shift reaction (WGS, CO + H2O → H2 + CO2), two essential processes to integrate fossil fuels toward a H2 energy loop, can be achieved on ZrO2/Cu­(111) catalysts near room temperature. Measurements of ambient-pressure X-ray photoelectron spectroscopy and mass spectrometry, combined with density functional calculations and kinetic Monte Carlo simulations, were used to study the behavior of the inverse oxide/metal catalysts. The superior performance is associated with a unique zirconia–copper interface, where multifunctional sites involving zirconium, oxygen, and copper work coordinatively to dissociate methane and water at 300 K and move forward the MWR and WGS processes.