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 CO₂ 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 H₂ even under infrared light irradiation. The open Ni sites are beneficial to capture and activate atmospheric CO₂ , while the photogenerated electrons dominate H₂ dissociation on the Pt sites. Simultaneously, thermal energy results in spilling of the dissociated H₂ 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.