Recently, simultaneously upgrading the greenhouse gas CO2 and underutilized ethane has introduced opportunities for synthesizing value-added industrial feedstocks. Depending on the selective bond cleavage in ethane, syngas (CO and H2) or ethylene can be produced via the dry reforming (C–C bond scission) and oxidative dehydrogenation (C–H bond scission) pathways, respectively. However, it remains challenging to identify and develop active sites responsible for the selective bond cleavage in ethane due to the structural and mechanistic complexities over 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 characterization and theoretical 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 the C–H bond to yield ethylene. This work identifies opportunities for using different interfacial structures in selectively upgrading abundant shale gas while mitigating greenhouse gas CO2.

Interfacial active sites for CO2-assisted selective cleavage of C–C/C–H bonds in ethane

ACS Spring Meeting 2021

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