The
extensive emission of CO2 into the atmosphere due
to the burning of fossil fuels has urged many countries to move toward
decarbonized energy. Based on the concept of carbon neutrality, the
European Union Emissions Trading System implemented the aviation carbon
tax (ACT), which stimulated the rapid transformation in aviation fuels.
To cope with the ACT and mitigate the CO2 emissions from
the aviation industry, here, we present a promising route for the
synthesis of precursors such as aromatics, alkyl benzenes, and naphthenes,
which account for 40–50 vol % fraction of the kerosene-based
aviation fuel, from waste CO2 or biomass-derived syngas.
The ultra-high selectivity of single-ring aromatics (precursors for
the kerosene-based aviation fuel) with a selective range of carbon
chain numbers (C8–C12) was achieved (>80%
in hydrocarbons at a reaction temperature of 275 °C) via the
catalytic hydrogenation of CO2 or CO over a bifunctional
catalyst (nano-sized ZnCr2O4/Sbx-H-ZSM-5). In
situ diffuse reflectance infrared Fourier transform spectroscopy,
Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy,
gas chromatography–mass spectrometry, and reaction analysis
revealed that the product distribution was controlled by thermodynamics
and the formation of the aromatics followed an “aldol–aromatic”
mechanism. The high selectivity of aromatics at the low reaction temperature
(i.e., 275 °C) was attributed to the catalyst topology, the closed
carbon chain aromatization reaction, and the presence of highly active
oxygenated species in the hydrocarbon pool. For the first time, an
asymmetric desorption behavior between the active oxygenate species
and aromatic hydrocarbons over the ZnCr2O4/Sbx-H-ZSM-5
catalyst is reported with the help of integrated differential phase
contrast scanning transmission electron microscopy, which made the
reaction highly selective toward aromatics. This strategy gives a
carbon-neutral route for the synthesis of kerosene-based aviation
fuel precursors and will reduce the burden of the carbon tax on the
aviation industry.