基于3-氨基-1,2,4-三氮唑配体的 MOF 催化 CO₂ 转化为环状碳酸酯.

黄羿杰; 王 静; 周家豪; 许周航; 邓栩生; 廖银念; 袁碧贞

CO2 is believed to be the main cause of rising global average surface temperatures and subsequent climate change. Converting carbon dioxide into chemicals through chemical processes is a powerful means of reducing its emissions and producing more economically valuable chemicals. The synthesis of cyclic carbonates from epoxides and CO2 stands out as a highly promising reaction due to its thermodynamically favorable nature and 100% atom economy. Among the diverse catalysts available for the catalytic conversion of CO2, metal-organic frameworks(MOFs) exhibit immense potential as multiphase catalysts. To enhance the performance of MOFs in CO2 fixation reactions, the modification of the pore surface through the incorporation of functional groups into the framework can be employed. In this study, based on 3-amino-1,2,4-triazolium ligands, a metal-organil framework material with simple preparation, structural stability and certain adsorption and activation function of CO2, Zn-Ataz-MOFs was synthesized to catalyze the conversion of CO2 and propylene oxide to produce propylene carbonate. Under the co-catalysis of 3%(mole fraction) Zn-Ataz-MOF and 2%(mole fraction) potassium iodide(KI) without solvent, the yield of propylene carbonate can reach 95% at 100℃ and 1 MPa CO2 pressure for 6 h, and the catalytic activity was still maintained after recycling for 5 times. The stability of the catalytic structure could be seen through structural characterization, and it has good substrate adaptability. The hypothesized mechanism is that the adsorption and activation of CO2 by Zn-Ataz-MOF and the synergistic catalysis of KI promote the efficient catalysis of the reaction.

CHEMICAL processes; PROPYLENE oxide; CATALYTIC activity; MOLE fraction; PROPYLENE carbonate; CARBON fixation

Journal of Molecular Science, 2023, Vol 39, Issue 5, p439

1000-9035

Academic Journal

10.13563/j.cnki.jmolsci.2023.18.102