Highly Active Au/δ-MoC and Cu/δ-MoC Catalysts for the Conversion of CO2: The Metal/C Ratio as a Key Factor Defining Activity, Selectivity, and Stability.
The ever growing increase of CO2 concentration in the atmosphere is one of the main causes of global warming. Thus, CO2 activation and conversion toward valuable added compounds is a major scientific challenge. A new set of Au/δ-MoC and Cu/δ-MoC catalysts exhibits high activity, selectivity, and stability for the reduction of CO2 to CO with some subsequent selective hydrogenation toward methanol. Sophisticated experiments under controlled conditions and calculations based on density functional theory have been used to study the unique behavior of these systems. A detailed comparison of the behavior of Au/β-Mo2C and Au/δ-MoC catalysts provides evidence of the impact of the metal/carbon ratio in the carbide on the performance of the catalysts. The present results show that this ratio governs the chemical behavior of the carbide and the properties of the admetal, up to the point of being able to switch the rate and mechanism of the process for CO2 conversion. A control of the metal/carbon ratio paves the road for an efficient reutilization of this environmental harmful greenhouse gas.
Departament de Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona , c/Martí i Franquès 1, 08028 Barcelona, Spain.
Sergio
S
Posada-Pérez
Facultad de Ciencias, Universidad Central de Venezuela , Caracas 1020-A, Venezuela.
Pedro J
PJ
Ramírez
Facultad de Ciencias, Universidad Central de Venezuela , Caracas 1020-A, Venezuela.
Jaime
J
Evans
Departament de Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona , c/Martí i Franquès 1, 08028 Barcelona, Spain.
Francesc
F
Viñes
Chemistry Department, Brookhaven National Laboratory , Upton, New York 11973, United States.
Ping
P
Liu
Departament de Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona , c/Martí i Franquès 1, 08028 Barcelona, Spain.
Francesc
F
Illas
Chemistry Department, Brookhaven National Laboratory , Upton, New York 11973, United States.
José A
JA
Rodriguez