The Reaction Mechanism Of The Acetylene Hydrochlorination On N-doped Graphene Catalyst

The non-mercury catalytic reaction of vinyl chloride is a promising catalyst forPVC production. In this paper, we use DFT (density function theory) to study theacetylene hydrochlorination reaction. Different valence states of gold species modelsare established to discuss their stability on different N-doped supports, and themechanism of the acetylene hydrochlorination on N-doped graphene catalyst andAu-based/graphene supports catalyst.The result shows favourable catalytic effect on acetylene hydrochlorination. Thecluster including Au,Au6Cl3and Au6Cl6have different valence state. With the valenceof Au ascending, the reaction paths have changed and the reaction barrier increased.After adsorbed on supports, the adsorption energy of Au chloride (Au2Cl6, Au2Cl2and Au2) becomes higher with the valence increasing. The N atom is doped into thegraphene, forming the pyridinic N-, the pyrrolic N-and the graphitic N-dopedgraphene. The results suggested that in the presence of the N-doped carbon supportcan enhance the stability of Au-based catalysts, in addition, pyridinic N is the mosteffective N-doped configuration.The N-doped carbon supports are also an excellent non-metal catalyst. The Natom has changed the electron density of graphene. As a result, the interactionbetween N-doped carbon supports and HCl turned to be stronger than that with C2H2，in case of the carbon deposition of catalysts caused by C2H2adsorption. During theadsorption, the HCl is attract more positive charge, which is in favour of electrophilicaddition reaction. The non-metal catalyst could save the use of precious metal andreduce production costs. The pyridinic N is also the most effective N-dopedconfiguration in non-metal cataly catalytic reaction.