Self- regeneration of Au/CeO 2 based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination

Abstract

Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactive sites. Here we show from synchrotron X-ray absorption, STEM imaging and DFT modelling that the availability of ceria(110) surface renders Au(0)/Au(I) as active pairs. Thus, Au(0) is directly involved in the catalysis. Owing to the strong mediating properties of Ce(IV)/Ce(III) with one electron complementary redox coupling reactions, the ceria promotion to Au catalysts gives enhanced activity and stability. Total pre-reduction of Au species to inactive Au nanoparticles of Au/CeO 2 &AC when placed in a C 2 H 2 /HCl stream can also rapidly rejuvenate. This is dramatically achieved by re-dispersing the Au particles to Au(0) atoms and oxidising to Au(I) entities, whereas Au/AC does not recover from the deactivation.