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Synergistic Interplay of Dual-Active-Sites on Metallic Ni-MOFs Loaded with Pt for Thermal-Photocatalytic Conversion of Atmospheric CO2 under Infrared Light Irradiation
Authors:Weimin Ma  Jingxue Sun  Shunyu Yao  Yutao Wang  Gang Chen  Guodong Fan  Yingxuan Li
Affiliation:1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 P. R. China

College of Chemistry and Chemical Engineering, Key Laboratory of Chemical Additives for China National Light Industry, Shaanxi University of Science and Technology, Xian, 710021 P. R. China

Contribution: Formal analysis (lead), ​Investigation (lead), Software (lead), Writing - original draft (lead);2. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 P. R. China;3. College of Chemistry and Chemical Engineering, Key Laboratory of Chemical Additives for China National Light Industry, Shaanxi University of Science and Technology, Xian, 710021 P. R. China

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.
Keywords:Atmospheric CO2 Capture  CO2 Conversion  Dual-Active-Sites  Metallic Pt/Ni-MOF  Thermal-Photocatalysis
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