FeK on 3D Graphene–Zeolite Tandem Catalyst with High Efficiency and Versatility in Direct CO2 Conversion to Aromatics

The direct conversion of CO2 with renewable H2 to aromatics can transform greenhouse gas and intermittent reproducible energies into valuable organic building blocks. However, the catalytic efficiency for this purpose remains low on existing catalysts containing either metal oxides (the methanol route) or iron (the olefin route) as the CO2 hydrogenation component(s). In this contribution, benefitting from the exceptional activity of the honeycomb-structured graphene (HSG)-supported, potassium-promoted iron (FeK1.5/HSG) in hydrogenating CO2 to light olefins, and with the help of the tandem HZSM-5, CO2 was converted to aromatics with a high selectivity of 41% among all the carbon-containing products (inclusive of CO) or 68% among all the hydrocarbons at a CO2 single-pass conversion of 35% and high space velocity of 26000 mL h–1 gcat–1, which results in an unprecedentedly high space time yield of aromatics of 11.8 μmolCO2 gcat–1 s–1. Furthermore, the dual-layer packing configuration of the FeK1.5/HSG-zeolite catalyst enables flexible adjustment of the aromatics spectrum simply by changing the type of the tandem zeolite. This work shows promise for the realization of a high-efficiency and versatile CO2-to-aromatics technology.