A DFT study of acetylene hydrogenation catalyzed by S-doped Pd1/g-C3N4

Abstract

To exploit the excellent properties of g-C3N4, more and more studies have been carried out in various fields in recent years to improve the selectivity of catalysts, especially for selective acetylene hydrogenation. To our best knowledge, Pd catalyst is of great importance to hydrogenate acetylene in ethylene feed. Though we have explored the hydrogenation of acetylene catalyzed by Pd1/g-C3N4 before, doping with non-metals has never been studied. In this work, the mechanisms of selective hydrogenation of acetylene to ethylene on S-doped Pd1/g-C3N4 were investigated and we also compared this result with undoped Pd1/g-C3N4. By comparing the activation energy and selectivity of undoped Pd1/g-C3N4 with those of S-doped C and N sites of Pd1/g-C3N4, we found that S-doped C sites can improve the reactivity, but with a poor selectivity, while the activity of S atom doped N sites was not improved, but the selectivity has improved. Our work provides significant insights to explore the development of high efficiency non-metallic doping single metal atoms supported on 2D layered materials.