Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane

Abstract

Summary Selective upgrading of underutilized ethane in shale gas with greenhouse gas CO2 can produce syngas via dry reforming (C–C bond scission) or ethylene via oxidative dehydrogenation (C–H bond scission). However, it remains challenging to identify active sites responsible for the selective bond cleavage in ethane due to the complexity of supported catalysts. Herein, the ethane-CO2 reaction over CeO2-supported catalysts was investigated to unravel the functions of distinct interfacial sites by combining kinetic measurements with in situ characterizations and calculations: the Pd/CeOx interface is responsible for supplying reactive oxygen species, electron-deficient oxygen species on Pd surface boosts the non-selective bond scission to produce syngas, electron-enriched oxygen in the FeOx/Pd interface enhances the selective scission of C–H bond to yield ethylene, and the FeOx/CeO2 interaction mediates oxygen supply and confines metal ensembles. The current work identifies opportunities for using different interfacial structures in upgrading abundant shale gas and CO2.