Natural Sunlight‐Driven CO₂ Hydrogenation into Light Olefins at Ambient Pressure over Bifunctional Cu‐Promoted CoFe Alloy Catalyst

Abstract The natural sunlight‐driven conversion of CO₂ into valuable C₂₊ products is urgently being pursued at ambient pressure, yet it poses a substantial challenge. Herein, a bifunctional Cu‐promoted CoFe alloy catalyst is designed for the natural light‐driven CO₂ hydrogenation into light olefins. Under a weak solar‐irradiation intensity of 0.45 kW m⁻² (0.45 sun), the optimal catalyst exhibits excellent activity and selectivity, with an impressive 73.7% selectivity for C₂₊ hydrocarbons and an outstanding 56.5% selectivity for C_2‐4 olefins, which is the best catalyst for C₂₊ hydrocarbons photosynthesis from natural sunlight to date. The bifunctional design of the catalyst combines the advantages of both metallic Cu and CoFe alloy components, providing a synergistic effect that enhances the CO₂ hydrogenation performance. The Cu promoter plays a crucial role in enhancing the adsorption of CO₂ and hydrogen spillover, while the CoFe alloy provides a stable coupling site of the C₁ intermediate for promoting the C_2‐4 olefins. This study provides new insights into the design of bifunctional catalysts for CO₂ hydrogenation and opens up new possibilities for sustainable production of light olefins from renewable resources.