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- W4313830464 abstract "This study investigated the effect of different alkaline earth metals doped La2-xMxCe2O7-δ (M = Ca, Sr, Ba and x = 0.30) catalysts prepared by one-step hydrothermal method for the low-temperature methane oxidative coupling (OCM) to olefins. The presence of a disordered cubic fluorite phase of synthesized catalysts was detected by powder XRD and Raman analysis. The surface analysis by XPS and Raman shows the presence of oxygen vacancy sites, which are responsible for the formation of electrophilic superoxide O2– species in presence of molecular oxygen. We observed that the ratio of active oxygen species (O2− and O22−) to lattice oxygen (O2–) was linearly correlated with the number of basic sites. The catalytic activity of different catalysts for the OCM reactions follows the order: La1.7Ca0.3Ce2O7-δ > La1.7Sr0.3Ce2O7-δ > La1.7Ba0.3Ce2O7-δ > La2Ce2O7. The reactivity order follows the same trend as the amount of basic sites and reactive oxygen species. According to this study, the best catalyst is La1.7Ca0.3Ce2O7-δ, which gives the highest C2 yield and C2 selectivity of 23.6 % and 78.8 %, respectively, at 650 °C. DFT studies revealed that substitution of La by Ca in the La2Ce2O7 catalyst significantly reduces the oxygen vacancy formation energy by about 100 kJ/mol compared to the undoped LaCe-oxide. We believe that the superior activity of La1.7Ca0.3Ce2O7-δ catalyst is attributed to the higher amount of basicity and electrophilic oxygen content, which are the governing factors in OCM for CH4 conversion and C2 product selectivity as well." @default.
- W4313830464 created "2023-01-09" @default.
- W4313830464 creator A5003911688 @default.
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- W4313830464 creator A5037090508 @default.
- W4313830464 date "2023-02-01" @default.
- W4313830464 modified "2023-10-13" @default.
- W4313830464 title "Enhancement of oxygen vacancy sites of La2-xMxCe2O7-δ (M = Ca, Ba, Sr) catalyst for the low temperature oxidative coupling of Methane: A combined DFT and experimental study" @default.
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