(239j) Effects of Doped N On the Reaction of Alkyne Hydrochlorination Catalyzed By Graphene Supported Au Based Catalyst

Many studies have shown that the support can greatly affect the distribution and stability of the catalyst through the interfacial interaction. It is a trend to modify the support to improve the catalytic performance. The aim of our work is to reveal the effect mechanism of the support modification by N-doping on the reaction of alkyne hydrochlorination catalyzed by graphene supported Au based catalyst. This investigation will provide a theoretical basis of how to select optimum N-doped location and valence state to interact with the catalyst and improve the catalytic performance. And it is instructive to the experimental design of novel non-mercury catalysts with high performance.

The graphene edge has two types: zigzag-edge and armchair-edge. Herein, four different N-doped sites are considered in this study: graphitic N, pyridine N on zigzag edge(zigzag 6-N), pyrrolic(armchair 5-N) and pyridine N(armchair 6-N) on armchair. Our results are divided into three sections:(a) The effects of doped N and its location on the stability of Au based catalyst. (b) The effects of doped N and its location on the adsorption of reactants and product. (c) The effects of doped N and its location on the reaction paths and barriers.