Artificial photosynthetic system for diluted CO2 reduction in gas-solid phase

Ya Wang, Jian-Xin Wei, Hong-Liang Tang, Lu-Hua Shao, Long-Zhang Dong, Xiao-Yu Chu, Yan-Xia Jiang, Gui-Ling Zhang, Feng-Ming Zhang () and Ya-Qian Lan ()
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Ya Wang: Harbin University of Science and Technology
Jian-Xin Wei: Harbin University of Science and Technology
Hong-Liang Tang: Harbin University of Science and Technology
Lu-Hua Shao: Harbin University of Science and Technology
Long-Zhang Dong: South China Normal University
Xiao-Yu Chu: Harbin University of Science and Technology
Yan-Xia Jiang: Harbin University of Science and Technology
Gui-Ling Zhang: Harbin University of Science and Technology
Feng-Ming Zhang: Harbin University of Science and Technology
Ya-Qian Lan: South China Normal University

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Rational design of robust photocatalytic systems to direct capture and in-situ convert diluted CO2 from flue gas is a promising but challenging way to achieve carbon neutrality. Here, we report a new type of host-guest photocatalysts by integrating CO2-enriching ionic liquids and photoactive metal-organic frameworks PCN-250-Fe2M (M = Fe, Co, Ni, Zn, Mn) for artificial photosynthetic diluted CO2 reduction in gas-solid phase. As a result, [Emim]BF4(39.3 wt%)@PCN-250-Fe2Co exhibits a record high CO2-to-CO reduction rate of 313.34 μmol g−1 h−1 under pure CO2 atmosphere and 153.42 μmol g−1 h−1 under diluted CO2 (15%) with about 100% selectivity. In scaled-up experiments with 1.0 g catalyst and natural sunlight irradiation, the concentration of pure and diluted CO2 (15%) could be significantly decreased to below 85% and 10%, respectively, indicating its industrial application potential. Further experiments and theoretical calculations reveal that ionic liquids not only benefit CO2 enrichment, but also form synergistic effect with Co2+ sites in PCN-250-Fe2Co, resulting in a significant reduction in Gibbs energy barrier during the rate-determining step of CO2-to-CO conversion.

Date: 2024
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DOI: 10.1038/s41467-024-53066-y

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