Conversion of CO 2 to value-added chemicals has been a long-standing objective, and direct hydrogenation of CO 2 to lower olefins is highly desirable but still challenging. Herein, we report a selective conversion of CO 2 to lower olefins through CO 2 hydrogenation over a ZnZrO/SAPO tandem catalyst fabricated with a ZnO-ZrO 2 solid solution and a Zn-modified SAPO-34 zeolite, which can achieve a selectivity for lower olefins as high as 80−90% among hydrocarbon products. This is realized on the basis of the dual functions of the tandem catalyst: hydrogenation of CO 2 on the ZnO-ZrO 2 solid solution and lower olefins production on the SAPO zeolite. The thermodynamic and kinetic coupling between the tandem reactions enable the highly efficient conversion of CO 2 to lower olefins. Furthermore, this catalyst is stable toward the thermal and sulfur treatments, showing the potential industrial application.
Hydrogenation of CO 2 to aromatics with selectivity of 73% among hydrocarbons at a single-pass conversion of 14% is achieved over a tandem catalyst. A thermodynamic coupling between CO 2 hydrogenation and aromatics formation was effectively conducted through the intermediate CH x O species. It was found that the presence of H 2 O and CO 2 not only facilitates aromatics production but also suppresses the formation of polycyclic aromatics, resulting in highly stable catalytic performance.
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