Density Functional Calculations on the Hydrogenation of Carbon Dioxide on Fe(111) and W(111) Surfaces

作者：Li Han Jung; Ho Jia Jen^*

来源：Journal of Physical Chemistry C, 2010, 114(2): 1194-1200.

DOI：10.1021/jp909428r

With quantum-chemical calculations, we investigated the hydrogenation of a CO(2) molecule on Fe(111) and W(111) surfaces using the density functional theory (DFT) with the projector-augmented wave (PAW) approach in periodic boundary condition. The structures and geometric parameters of the hydrogenation products, and the potential-energy surfaces, were calculated. It was shown that similar reaction paths for the hydrogenation of CO(2) on Fe(111) and W(111) surfaces were found but with disparate energies. The rate-controlling energy barriers from M-CO(2) (M = Fe, W) Plus H atom to form formate (HCOO) and carboxyl (COOH) on a Fe(111) surface are 0.37 and 1.69 eV, respectively, but 0.54 and 2.79 eV, respectively, oil a W(111) Surface. The most probable path for the hydrogenation of a CO(2) molecule on either the Fe(111) or W(111) surface is the formation of formate-vertical structure. To understand the interaction between adsorbates and surfaces, we Calculated the Bader charges and analyzed the local densities of states.

• 出版日期2010-1-21