Crystal Engineering of MOF‐Derived Bimetallic Oxide Solid Solution Anchored with Au Nanoparticles for Photocatalytic CO2 Reduction to Syngas and C2 Hydrocarbons

Abstract Considering that CO 2 reduction is mostly a multielectron reaction, it is necessary for the photocatalysts to integrate multiple catalytic sites and cooperate synergistically to achieve efficient photocatalytic CO 2 reduction to various products, such as C 2 hydrocarbons. Herein, through crystal engineering, we designed and constructed a metal–organic framework‐derived Zr/Ti bimetallic oxide solid solution support, which was confirmed by X‐ray diffraction, electron microscopy and X‐ray absorption spectroscopy. After anchoring Au nanoparticles, the composite photocatalyst exhibited excellent performances toward photocatalytic CO 2 reduction to syngas (H 2 and CO production rates of 271.6 and 260.6 μmol g −1 h −1 ) and even C 2 hydrocarbons (C 2 H 4 and C 2 H 6 production rates of 6.80 and 4.05 μmol g −1 h −1 ). According to the control experiments and theoretical calculations, the strong interaction between bimetallic oxide solid solution support and Au nanoparticles was found to be beneficial for binding intermediates and reducing CO 2 reduction, highlighting the synergy effect of the catalytic system with multiple active sites.