Intermediate Product Regulation in Tandem Solid Catalysts with Multimodal Porosity for High‐Yield Synthetic Fuel Production

Tandem catalysis is an attractive strategy to intensify chemical technologies. However, simultaneous control over the individual and concerted catalyst performances poses a challenge. We demonstrate that enhanced pore transport within a Co/Al 2 O 3 Fischer–Tropsch (FT) catalyst with hierarchical porosity enables its tandem integration with a Pt/ZSM‐5 zeolitic hydrotreating catalyst in a spatially distant fashion that allows for catalyst‐specific temperature adjustment. Nevertheless, this system resembles the case of close active‐site proximity by mitigating secondary reactions of primary FT α‐olefin products. This approach enables the combination of in situ dewaxing with a minimum production of gaseous hydrocarbons (18 wt %) and an up to twofold higher (50 wt %) selectivity to middle distillates compared to tandem pairs based on benchmark mesoporous FT catalysts. An overall 80 % selectivity to liquid hydrocarbons from syngas is attained in one step, attesting to the potential of this strategy for increasing the carbon efficiency in intensified gas‐to‐liquid technologies.