The oriented conversion of CO2 into target high‐value chemicals is an effective way to reduce carbon emissions, but still presents a challenge. In this communication, we report the oriented conversion of CO2 into value‐added aromatics, especially para‐xylene, in a single pass by combining core–shell structured Zn‐doped H‐ZSM‐5 (Zn‐ZSM‐5@SiO2) and a Cr2O3 component. Through precise regulation of the acidity of Zn‐ZSM‐5@SiO2, high para‐xylene selectivity (38.7 % in the total products) at a CO2 conversion of 22.1 % was achieved. Furthermore, a CO2‐assisted effect in the synthesis of aromatics during the tandem process has been clarified through a control experiment. The CO2 reactant can act as a hydrogen acceptor to accelerate the dehydrogenation of alkenes, intermediates in the synthesis of aromatics, thereby increasing the driving force towards aromatics in the tandem reaction process.
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