Selective Photocatalytic Reduction of CO2 to CO Mediated by Silver Single Atoms Anchored on Tubular Carbon Nitride |
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| Authors: | Dr Shan Hu Dr Panzhe Qiao Dr Xinli Yi Yiming Lei Huilin Hu Prof Jinhua Ye Prof Defa Wang |
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| Institution: | 1. TJU–NIMS International Collaboration Laboratory, Key Laboratory of Advanced Ceramics and Machining Technology (Ministry of Education) and Tianjin Key Laboratory of Composite and Functional Materials, School of Material Science and Engineering, Tianjin University, 300072 Tianjin, China;2. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201204 Shanghai, China;3. College of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, 443002 Yichang, China |
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| Abstract: | Artificial photosynthesis is a promising strategy for converting carbon dioxide (CO2) and water (H2O) into fuels and value-added chemical products. However, photocatalysts usually suffered from low activity and product selectivity due to the sluggish dynamic transfer of photoexcited charge carriers. Herein, we describe anchoring of Ag single atoms on hollow porous polygonal C3N4 nanotubes (PCN) to form the photocatalyst Ag1@PCN with Ag−N3 coordination for CO2 photoreduction using H2O as the reductant. The as-synthesized Ag1@PCN exhibits a high CO production rate of 0.32 μmol h−1 (mass of catalyst: 2 mg), a high selectivity (>94 %), and an excellent stability in the long term. Experiments and density functional theory (DFT) reveal that the strong metal–support interactions (Ag−N3) favor *CO2 adsorption, *COOH generation and desorption, and accelerate dynamic transfer of photoexcited charge carriers between C3N4 and Ag single atoms, thereby accounting for the enhanced CO2 photoreduction activity with a high CO selectivity. This work provides a deep insight into the important role of strong metal–support interactions in enhancing the photoactivity and CO selectivity of CO2 photoreduction. |
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| Keywords: | C3N4 CO2 Photoreduction Metal–Support Interaction Silver Single-Atom Catalyst |
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