Single-Atom X/g-C3N4(X = Au1, Pd1, and Ru1) Catalysts for Acetylene Hydrochlorination: A Density Functional Theory Study

The mechanisms of the single-atom X/g-C3N4(X = Au-1, Pd-1, and Ru-1) catalysts for the acetylene hydrochlorination reaction were systematically investigated using the density functional theory (DFT) B3LYP method. The density functional dispersion correction obtained by the DFT-D3 method was taken into account. During the reaction, C2H2 and HCl were well activated and the analysis of the adsorption energy demonstrated the adsorption performance of C2H2 is better than that of HCl. The catalytic mechanisms of the three catalysts consist of one intermediate and two transition states. Moreover, our results showed that the three single-atom catalysts improve the catalytic activity of the reaction to different degrees. The calculated energy barrier declines in the order of Pd-1/g-C3N4 > Ru-1/g-C3N4 > Au-1/g-C3N4, and the energy barrier for the Au-1/g-C3N4 catalyst was only 13.66 kcal/mol, proving that single-atom Au-1/g-C3N4 may be a potential catalyst for hydrochlorination of acetylene to vinyl chloride.