Theoretical study of reactivity of gold clusters: Structural effects and support effects

In this talk, we focus on catalytic activity of gold nano-clusters from the viewpoints of structural effects and support effects. The enormous interest in nanocatalysis is stipulated by the fact that the catalytic activity of nano-clusters strongly depends on their size, structure, morphology, charge state, type of the support material, etc., and hence can be controlled and tuned by these factors. Despite intensive theoretical and experimental studies, clear understanding of the morphology effects in nanocatalysis is still lacking. Metal clusters are structural flexible, meaning that they possess different structures and different reactivity for the same sized cluster. Recently, we proposed a novel effective strategy for a systematic search of single bond activation reaction by small metal clusters [1-3], using the artificial force-induced reaction method [4]. The results demonstrated that the most stable structure of metal clusters are not always highly reactive and the most stable adsorption configurations of reactants on metal clusters do not necessarily lead to the low-barrier dissociation pathways. Therefore, in order to investigate the activity of metal clusters, the contribution of all the possible reaction sites and low-energy isomers are highly required.

REFERENCES
[1] M. Gao, A. Lyalin, S. Maeda, and T. Taketsugu, J. Chem. Theo. Comp., 2014, 10, 1623-1630.
[2] M. Gao, A. Lyalin, M. Takagi, S. Maeda, and T. Taketsugu, J. Phys. Chem. C, 2015, 119, 11120-11130.
[3] M. Gao, D. Horita, Y. Ono, A. Lyalin, S. Maeda, and T. Taketsugu, J. Phys. Chem. C, 2017, 121, 2661-2668.
[4] S. Maeda, Y. Harabuchi, M. Takagi, T. Taketsugu and K. Morokuma, Chem. Rec., 2016, 16, 2232−2248.