Methane carbonylation to light olefins and alcohols over carbon–based iron– and cobalt–oxide catalysts

Abstract

Herein, iron– [Fe] and cobalt–oxide [Co] nanoparticles supported on carbon were synthesized through the construction of the co-assembly strategy via the mixture of carbon source resol, diglyme, triblock copolymer, and M(acac)x (M = Fe3+ and Co2+) complexes. The prepared nanocomposites possess large pore sizes, high surface areas, large pore volumes, and highly dispersed nanoparticles. The exceptional catalytic performance together with high selectivity toward alcohol and light olefin products over the [Fe] and [Co] catalysts were observed in the CH4 carbonylation reaction. The [Fe] catalyst displayed an acceptable CH4 conversion of 40% and high selectivity toward C2–C4 light olefins (>42%) and C1–C4 alcohols (>38%) while exhibiting a low CO2 production at moderate CO conversion of >52%. The CH4 conversion was lower over the [Co] catalyst, although the selectivity of alcohols stretched beyond the [Fe] catalyst (~76%), with CH4 and CO conversion of 15.40 and 31.83%, respectively. Besides alcohol, low acetic acid and ethanal (acetaldehyde) formed over the [Co] catalyst. The catalysts were also employed in the Fischer–Tropsch synthesis (FTS). The [Fe] catalyst demonstrated high FTS catalytic performance with 85% CO conversion, the high C2–C4 selectivity, and low selectivity of methane. In comparison, the [Co] catalyst exhibited high conversion of CO (>81%) and suitable selectivity toward C2–C4 and C5+ hydrocarbons.