Graphical Abstract

CO2-assisted oxidative dehydrogenation of ethane (CO2-ODHE) and dry reforming of ethane (DRE) have provided a promising way to simultaneously upgrade CO2 and ethane to produce value-added industrial feedstocks, such as syngas (CO and H2), or ethylene. CeO2-supported Pd bimetallic catalysts have been demonstrated to be efficient catalysts for these reactions. In particular, the Pd-O-Ce interface and Pd-O-Fe (or Pd-O-In) interface were verified as the key active sites for producing syngas and ethylene, respectively. However, how to regulate the amount of interface to further enhance the product yield is still a major challenge in this area. In this study, we show that the ratio of the Pd-O-Ce interface can be optimized through the CeO2 nano-island strategy. CeO2 nano-islands with different loadings and sizes are grafted onto the high-surface-area SiO2, and are then used for anchoring PdFen bi-metals, thus leading to the formation of interfaces with different amounts of Pd-O-Ce. The results show that when the Ce loading reaches 15 wt%, the supported PdFen catalyst has the highest ratio at the Pd-O-Ce interface, resulting in a significant increase in the syngas yield (879.1μmol · g-1 · min-1for CO and 508.1μmol · g-1 · min-1 for H2 respectively), which is the best among all the reported state-of-the-art catalysts in the literature. At the same time, the ethylene production rate can be maintained at a high level of 172.5 μmol · g-1 · min-1.