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 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.

Carbon Dots Anchoring Single-Atom Pt on C3N4 Boosting Photocatalytic Hydrogen Evolution

“…H 2 -temperature programmed desorption (H 2 -TPD) (Figure 5b) further reveals the interaction between Pt species and C 3 N 4 . The reduction temperature of Pt species in Pt-CDs/C 3 N 4 (152 • C) is higher than that of Pt-C 3 N 4 (121.6 • C), demonstrating that the interaction between Pt species and CDs/C 3 N 4 is stronger than C 3 N 4 , which greatly stabilizes the Pt species to form the single-atom structures [37,38]. The change in Pt particle sizes is mainly due to the introduction of CDs, which can effectively anchor small-sized Pt metal onto C3N4.…”