Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites

Abstract

Abstract Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H2 at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 oC, and a record space-time yield of ethylene of 1123 molC2H4 molPd −1 h−1 under ambient conditions, which is nearly four times that of the typical Pd1Ag3/Al2O3 catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pdδ+, which not only facilitates C2H2 hydrogenation but also promotes C2H4 desorption, thereby enabling a high conversion of C2H2 to C2H4 at room temperature while suppressing over-hydrogenation to C2H6.