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

被引：41

作者：

Wang, Ya ^{[1
]}

Wei, Jian-Xin ^{[1
]}

Tang, Hong-Liang ^{[1
]}

Shao, Lu-Hua ^{[1
]}

Dong, Long-Zhang ^{[2
]}

Chu, Xiao-Yu ^{[1
]}

Jiang, Yan-Xia ^{[1
]}

Zhang, Gui-Ling ^{[1
]}

Zhang, Feng-Ming ^{[1
]}

Lan, Ya-Qian ^{[2
]}

机构：

[1] Harbin Univ Sci & Technol, Sch Mat Sci & Chem Engn, Heilongjiang Prov Key Lab CO2 Resource Utilizat &, Harbin 150080, Heilongjiang, Peoples R China

[2] South China Normal Univ, Sch Chem, Guangzhou 510006, Peoples R China

来源：

NATURE COMMUNICATIONS | 2024年 / 15卷 / 01期

基金：

中国博士后科学基金; 中国国家自然科学基金;

关键词：

MOLECULAR-ORBITAL METHODS; TOTAL-ENERGY CALCULATIONS; METAL-ORGANIC FRAMEWORK; EFFICIENT; PHOTOCATALYST; CLUSTERS;

D O I：

10.1038/s41467-024-53066-y

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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(39.3wt%)@PCN-250-Fe2Co exhibits a record high CO2-to-CO reduction rate of 313.34 mu mol g(-1) h(-1) under pure CO2 atmosphere and 153.42 mu mol g(-1) h(-1) under diluted CO2 (15%) with about 100% selectivity. In scaled-up experiments with 1.0g 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.

引用

页数：13

共 75 条

[1] Efficient Visible-Light Photoreduction of CO2 to CH4 over an Fe-Based Metal-Organic Framework (PCN-250-Fe3) in a Solid-Gas Mode [J].