Lawrence Berkeley National Laboratory

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.