Tandem Catalysis for CO<sub>2</sub> Hydrogenation to C<sub>2</sub>–C<sub>4</sub> Hydrocarbons

Conversion of carbon dioxide to C<sub>2</sub>–C<sub>4</sub> 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 CeO<sub>2</sub>–Pt@mSiO<sub>2</sub>–Co for converting CO<sub>2</sub> to C<sub>2</sub>–C<sub>4</sub> hydrocarbons using two metal-oxide interfaces. C<sub>2</sub>–C<sub>4</sub> 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/CeO<sub>2</sub> interface converts CO<sub>2</sub> and H<sub>2</sub> to CO, and on the neighboring Co/mSiO<sub>2</sub> interface yields C<sub>2</sub>–C<sub>4</sub> hydrocarbons through a subsequent Fischer–Tropsch process. In addition, the catalysts show no obvious deactivation over 40 h. The successful production of C<sub>2</sub>–C<sub>4</sub> 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.