Defect-Dependent Selective C–H/C–C Bond Cleavage of Propane in the Presence of CO<sub>2</sub> over FeNi/Ceria Catalysts
Yehong Wang, Zhixin Zhang, Lijun Lei, Wen Liu, Shuyan Du, Xiangxue Zhu, Xiujie Li, Feng Wang
Abstract
CO2-assisted propane conversion is one of the most interesting chemical processes, generating either propylene via C–H bond cleavage or syngas via C–C bond cleavage of propane. However, controlling the conversion with high selectivity is still a significant challenge. In this work, we developed a strategy to realize selective C–H/C–C bond cleavage of propane with CO2 as the oxidant by controlling the defect concentrations of ceria supports over FeNi/ceria catalysts. Two types of ceria with distinct defect concentrations were prepared successfully. The propane conversion achieved 25.2% with 49% propylene selectivity via C–H bond cleavage over the defect-rich ceria-supported FeNi catalyst at 550 °C. In contrast, CO is generated via C–C bond cleavage with 95% selectivity when defect-deficient ceria was used as the support. The essential role of defects in the ceria support was investigated carefully by UV–Raman, X-ray photoelectron spectroscopy, and H2-temperature-programmed reduction. This work provides a method for defect tuning of ceria-based catalysts and realizes the selective conversion of CO2 and alkanes to value-added chemicals.