能機理性地探討結構、配體與合體效應在非均相催化反應的影響(2/2)

The experimental observation, which found that the reactivity for methanol decomposition can be improved on annealed Rh clusters, has been mechanistically elucidated by the density functional theory (DFT) based computation, as detailed in the present report. The reactivity of methanol decomposition directly corresponds to the structures of Rh clusters, in which the low-coordinated Rh atoms on the surface can tighten the methanol adsorption to avoid its desorption and assist the bond dissociation to speed up the decomposition, as detailed in our previous study. Thus, the improved reactivity of annealed Rh cluster can be attributable to the structure change of Rh cluster due to annealing. We computationally examined the thermodynamic stability of several Rh clusters on θ-Al2O3(100) and Rh(100) surfaces in the experimental condition to investigate the annealing effect on the structural change. Furthermore, we utilized MD simulation to find the structure evolution of Rh clusters in the annealing process.