A Stacked Plasmonic Metamaterial with Strong Localized Electric Field Enables Highly Efficient Broadband Light-Driven CO 2 Hydrogenation.

Light utilization largely governs the performance of CO 2 photoconversion, whereas most of the materials that are implemented in such an application are restricted in a narrow spectral absorption range. Plasmonic metamaterials with a designable regular pattern and facile tunability are excellent candidates for maximizing light absorption to generate substantial hot electrons and thermal energy. Herein, a concept of coupling a Au-based stacked plasmonic metamaterial with single Cu atoms in alloy, as light absorber and catalytic sites, respectively, is reported for gas-phase light-driven catalytic CO 2 hydrogenation. The metamaterial structure works in a broad spectral range (370-1040 nm) to generate high surface temperature for photothermal catalysis, and also induces strong localized electric field in favor of transfer of hot electrons and reduced energy barrier in CO 2 hydrogenation. This work unravels the significant role of a strong localized electric field in photothermal catalysis and demonstrates a scalable fabrication approach to light-driven catalysts based on plasmonic metamaterials.