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

Infrared light driven photocatalytic reduction of atmospheric CO(2 )is challenging due to the ultralow concentration of CO2 (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 CO2 with H-2 even under infrared light irradiation. The open Ni sites are beneficial to capture and activate atmospheric CO2, 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 CO2 is thermally reduced to CO and CH4. The synergistic interplay of dual-active-sites renders Pt/Ni-MOF a record efficiency of 9.57 % at 940 nm for converting atmospheric CO2, enables the procurement of CO2 to be independent of the emission sources, and improves the energy efficiency for trace CO2 conversion by eliminating the capture media regeneration and molecular CO2 release.