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

Rational design of robust photocatalytic systems to direct capture and in-situ convert diluted CO 2 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 CO 2 -enriching ionic liquids and photoactive metal-organic frameworks PCN-250-Fe 2 M (M = Fe, Co, Ni, Zn, Mn) for artificial photosynthetic diluted CO 2 reduction in gas-solid phase. As a result, [Emim]BF 4 (39.3 wt%)@PCN-250-Fe 2 Co exhibits a record high CO 2 -to-CO reduction rate of 313.34 μmol g −1 h −1 under pure CO 2 atmosphere and 153.42 μmol g −1 h −1 under diluted CO 2 (15%) with about 100% selectivity. In scaled-up experiments with 1.0 g catalyst and natural sunlight irradiation, the concentration of pure and diluted CO 2 (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 CO 2 enrichment, but also form synergistic effect with Co 2+ sites in PCN-250-Fe 2 Co, resulting in a significant reduction in Gibbs energy barrier during the rate-determining step of CO 2 -to-CO conversion. Artificial photosynthetic diluted CO 2 reduction from fuel gas is promising but challenging for carbon neutrality. Here, the authors report a host-guest system by integrating CO 2 -enriching ionic liquids and photoactive metal-organic frameworks, greatly enhancing CO 2 -to-CO conversion efficiency.