Tandem Catalysis for CO₂ Hydrogenation to C₂–C₄ Hydrocarbons

Abstract

Conversion of carbon dioxide to C₂-C₄ hydrocarbons is a major pursuit in clean energy research. Despite tremendous efforts, the lack of well-defined catalysts in which the spatial arrangement of interfaces is precisely controlled hinders the development of more efficient catalysts and in-depth understanding of reaction mechanisms. Herein, we utilized the strategy of tandem catalysis to develop a well-defined nanostructured catalyst CeO₂-Pt@mSiO₂-Co for converting CO₂ to C₂-C₄ hydrocarbons using two metal-oxide interfaces. C₂-C₄ hydrocarbons are found to be produced with high (60%) selectivity, which is speculated to be the result of the two-step tandem process uniquely allowed by this catalyst. Namely, the Pt/CeO₂ interface converts CO₂ and H₂ to CO, and on the neighboring Co/mSiO₂ interface yields C₂-C₄ hydrocarbons through a subsequent Fischer-Tropsch process. In addition, the catalysts show no obvious deactivation over 40 h. The successful production of C₂-C₄ hydrocarbons via a tandem process on a rationally designed, structurally well-defined catalyst demonstrates the power of sophisticated structure control in designing nanostructured catalysts for multiple-step chemical conversions.