Novel nitrogen-doped Au-embedded graphene single-atom catalysts for acetylene hydrochlorination: A density functional theory study

Abstract

Abstract The mechanisms of an Au-embedded graphene (AuG) single-atom catalyst (SAC) and AuG-SACs doped with nitrogen at different locations for acetylene hydrochlorination were investigated through density functional theory (DFT). The density functional dispersion correction was calculated with the DFT-D3 method. We studied the adsorption characteristics of HCl and C2H2 on these SACs and simulated the corresponding reaction mechanism. We also found that adding the heteroatom N to AuG-SACs can reduce the reaction activation energy. Furthermore, we found the optimal location of the N atom of the N–substituted SAC to reduce the activation energy. The results suggest that N-doped AuG-SACs could find potential in catalyzing acetylene hydrochlorination to vinyl chloride and reduce the amount of noble metal used in mercury-free catalysts.