Abstract
Ethylene in principle can be obtained via oxidative coupling of methane (OCM), but it is urgently calling for a low-temperature active and selective catalyst. To accomplish this goal, the CexZr1-xO2 solid solutions with varied Ce/Zr molar ratio were modified with Mn2O3-Na2WO4 to fabricate OCM catalysts. The effects of Ce/Zr ratio and Mn2O3-Na2WO4 doping were investigated on the catalyst reactivity for the OCM, showing that the reaction light-off temperature, activity and selectivity are subject to the Ce/Zr molar ratio and Mn2O3-Na2WO4 doping. The promising catalyst with Ce/Zr molar ratio of 0.15/0.85 achieves 25% CH4 conversion with 67% selectivity to C2-C3 at 660 °C and is stable for at least 100 h. The catalysts were systematically studied by CH4-TPSR, O2-TPO/-TPD, CH4-pulse, in-situ FT-IR, EPR and XPS, showing that the Mn2O3-Na2WO4 doped Ce0.15Zr0.85O2 can generate more O2– species thereby leading to a markedly improved activity and selectivity at much lowered reaction temperature.
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