Synergistic Interplay of Dual‐Active‐Sites on Metallic Ni‐MOFs Loaded with Pt for Thermal‐Photocatalytic Conversion of Atmospheric CO2 under Infrared Light Irradiation

Abstract Infrared light driven photocatalytic reduction of atmospheric CO 2 is challenging due to the ultralow concentration of CO 2 (0.04 %) and the low energy of infrared light. Herein, we develop a metallic nickel‐based metal–organic framework loaded with Pt (Pt/Ni‐MOF), which shows excellent activity for thermal‐photocatalytic conversion of atmospheric CO 2 with H 2 even under infrared light irradiation. The open Ni sites are beneficial to capture and activate atmospheric CO 2 , while the photogenerated electrons dominate H 2 dissociation on the Pt sites. Simultaneously, thermal energy results in spilling of the dissociated H 2 to Ni sites, where the adsorbed CO 2 is thermally reduced to CO and CH 4 . The synergistic interplay of dual‐active‐sites renders Pt/Ni‐MOF a record efficiency of 9.57 % at 940 nm for converting atmospheric CO 2 , enables the procurement of CO 2 to be independent of the emission sources, and improves the energy efficiency for trace CO 2 conversion by eliminating the capture media regeneration and molecular CO 2 release.