Abstract

Elucidation of the intrinsic catalytic principle of iron carbides remains a substantial challenge in iron-catalyzed Fischer-Tropsch synthesis (FTS), due to possible interference from other Fe-containing species. Here, we propose a facile approach to synthesize single-phase θ-Fe3C via the pyrolysis of a molecularly defined Fe-C complex (Fe4[Fe(CN)6]3), thus affording close examination of its catalytic behavior during FTS. The crystal structure of prepared θ-Fe3C is unambiguously verified by combined XRD and MES measurement, demonstrating its single-phase nature. Strikingly, single-phase θ-Fe3C exhibited excellent selectivity to light olefins (77.8%) in the C2-C4 hydrocarbons with less than 10% CO2 formation in typical FTS conditions. This strategy further succeeds with promotion of Mn, evident for its wide-ranging compatibility for the promising industrial development of catalysts. This work offers a facile approach for oriented preparation of single-phase θ-Fe3C and provides an in-depth understanding of its intrinsic catalytic performance in FTS.

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