摘要
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 Ce x Zr 1-x O 2 solid solutions with varied Ce/Zr molar ratio were modified with Mn 2 O 3 -Na 2 WO 4 to fabricate OCM catalysts. The effects of Ce/Zr ratio and Mn 2 O 3 -Na 2 WO 4 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 Mn 2 O 3 -Na 2 WO 4 doping. The promising catalyst with Ce/Zr molar ratio of 0.15/0.85 achieves 25% CH 4 conversion with 67% selectivity to C 2 -C 3 at 660 °C and is stable for at least 100 h. The catalysts were systematically studied by CH 4 -TPSR, O 2 -TPO/-TPD, CH 4 -pulse, in-situ FT-IR, EPR and XPS, showing that the Mn 2 O 3 -Na 2 WO 4 doped Ce 0.15 Zr 0.85 O 2 can generate more O 2 – species thereby leading to a markedly improved activity and selectivity at much lowered reaction temperature.
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