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

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 + 3H(2)) and the water-gas shift reaction (WGS, CO + H2O?H-2 + 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.

Automated summary

Enzymatic systems have been found to catalytically convert methane at room temperature under mild conditions. This study demonstrates that the reforming of methane by water and the water-gas shift reaction can be achieved on ZrO2/Cu(111) catalysts near room temperature. The superior performance of the catalyst is attributed to a unique zirconia-copper interface, where multifunctional sites involving zirconium, oxygen, and copper work together to dissociate methane and water, facilitating the desired reactions.