A DFT Study of Methanol Synthesis from CO2 Hydrogenation on the Pd(111) Surface

作者：Zhang, Minhua; Wu, Yufei; Dou, Maobin; Yu, Yingzhe^*

来源：Catalysis Letters, 2018, 148(9): 2935-2944.

DOI：10.1007/s10562-018-2497-y

• Pd(111)
• CO2 hydrogenation
• Methanol synthesis
• Density functional theory

During the process of catalytic conversion of -CO2 to valuable chemical products, Pd used as catalysts or modifiers shows promising effect on -CO2 hydrogenation. The mechanism of methanol synthesis from the hydrogenation of -CO2 on the Pd(111) surface was studied using density functional theory calculations in present work. On the Pd(111) surface, -CO2 firstly hydrogenates to HCOO or COOH, each of which then reacts with the surface H atom to form HCOOH. Next, HCOOH dissociates to OH and HCO that will be consecutively hydrogenated to -H2CO, -H3CO and -H3COH. CO is the main side product of -CO2 hydrogenation on the Pd(111) surface with an activation barrier of 1.09 eV. The hydrogenation of HCO species with the surface H atom to form -H2CO plays as the rate determining step for -CO2 hydrogenation to methanol with the barrier of 0.91 eV. Our calculated results are favorable for the understanding of the mechanism of -CO2 conversion on not only Pd-based catalysts but also Pd modified catalysts. Graphical Abstract The mechanism of methanol synthesis from the hydrogenation of -CO2 on the Pd(111) surface was studied using density functional theory calculations.
[GRAPHICS]
.

• 出版日期2018-9
• 单位天津大学