Effect of catalyst preparation and storage on chemical looping epoxidation of ethylene

Abstract

Chemical looping epoxidation (CLE) of ethylene to ethylene oxide (EO) presents an exciting alternative to the incumbent technology of direct epoxidation of ethylene with O2(g). In CLE, the reaction is still catalysed by Ag but oxygen is provided as Olattice from a solid metal oxide, eliminating the need and limitations of using O2(g). Here, the influence of catalyst preparation in CLE is investigated. The Ag catalyst was impregnated on a solid oxide, SrFeO3, which was used as the donor of Olattice in CLE. Temperature programmed reduction in H2 indicated that O-species participating in CLE can be attributed to the removal of the first monolayer of oxygen in SrFeO3. By changing the temperature of calcination in Ag-SrFeO3 preparation, the size of Ag particles was varied, resulting in a simultaneous increase of selectivity for EO (up to 60%) and conversion of C2H4 (up to 10%). Then, an assessment of the effects of impurities (carbonates, hydroxides), which deposit over time on the Ag-SrFeO3 surface, was performed, showing that impurities deteriorate the catalyst performance in CLE. Finally, the doping of the SrFeO3 with Ce to the A-site of the perovskite was carried out, and a substantial improvement of the conversion of C2H4 was achieved, reaching 15%, while maintaining the 60% selectivity for EO.