Oxidative dehydrogenation and dry reforming of n-butane with CO2 over NiFe bimetallic catalysts
2018
Abstract The oxidative dehydrogenation of n -butane to 1,3-butadiene using CO 2 as a soft oxidant is investigated over oxide-supported NiFe bimetallic catalysts. Dry reforming of n -butane with CO 2 to syngas is also studied under identical conditions for comparison. The Ni 1 Fe 3 /CeO 2 catalyst is identified as a promising catalyst for the oxidative dehydrogenation to 1,3-butadiene via the C H bond cleavage, while the Ni 3 Fe 1 /CeO 2 catalyst mainly promotes the dry reforming pathway via the C C bond scission. The oxidation states of Ni and Fe are determined by X-ray absorption fine structure (XAFS) measurements under reaction conditions. Density functional theory (DFT) calculations are performed to further understand the different reaction pathways. Furthermore, the effect of oxide supports is studied for the Ni 1 Fe 3 bimetallic catalysts, showing that highly reducible supports, CeO 2 and CeO 2 -ZrO 2 , promote the production of 1,3-butadiene, whereas the ZrO 2 support significantly suppresses the oxidative dehydrogenation.
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