A DFT study of graphene-FeNx (x = 4, 3, 2, 1) catalysts for acetylene hydrochlorination

In this paper, we used density functional theory (DFT) to systematically study the mechanism and activity of a graphene-FeNx (x = 4, 3, 2, 1) series of non-noble metal catalysts for acetylene hydrochlorination at the B3LYP/6–31 G** level, and the LANL2DZ effective core pseudo-potentials basis set was applied to Fe atom. Dispersion-corrected DFT-D3 was considered in the calculation. In the process of the graphene-FeNx catalytic reaction, all the catalysts adsorbed acetylene first and adsorbed hydrogen chloride later to form a co-adsorption structure. The calculation results displayed that with a decrease in doped nitrogen atoms in the catalyst, the activity of the reaction decreased successively. Graphene-FeN4 showed excellent catalytic performance, and its energy barrier was only 16.80 kcal/mol. Accordingly, it is a latent non-noble metal catalyst for hydrochlorination of acetylene. [Display omitted] •The mechanisms of non-noble metal graphene-FeNx (x= 4, 3, 2, 1) catalysts for acetylene hydrochlorination were investigated.•The mechanisms of these catalysts were found to be similar.•Graphene-FeN4 is a potential catalyst for acetylene hydrochlorination.