Bera Priti, Sundari Kalimuthu Abirami, Karthik Veerappan, Das Pritam, Cha Pil-Ryung, Dhakshinamoorthy Amarajothi, Biswas Shyam
Department of Chemistry, Indian Institute of Technology Guwahati, Guwahati 781039, Assam, India.
School of Chemistry, Madurai Kamaraj University, Madurai 625021, Tamil Nadu, India.
Inorg Chem. 2025 Jul 28;64(29):15078-15087. doi: 10.1021/acs.inorgchem.5c01963. Epub 2025 Jul 14.
Carbon dioxide (CO) is a major greenhouse gas that poses serious environmental and health risks. Converting CO into valuable chemicals or fuels offers a sustainable solution to reducing fossil fuel dependence. Metal-organic frameworks (MOFs) are efficient catalysts in CO cycloaddition due to their porosity, nitrogen-rich ligands, and dual Lewis acid-base active sites, enhancing catalytic efficiency and enabling efficient CO utilization. Therefore, we designed a stable microporous MOF with a nitrogen-rich ligand. This activated MOF () demonstrates exceptional stability and high surface area, which is effective for the adsorption of CO molecules into its pore. The use of efficiently converts CO and epoxides into cyclic carbonates under moderate conditions, exhibiting an excellent catalytic performance. Catalyst showed outstanding catalytic activity even after a fourth cycle with a minimal loss of its efficiency. Furthermore, the catalytic performance of was also tested in the Friedel-Crafts alkylation of indole with β-nitrostyrene in toluene using as a catalyst. The solid retained its activity over four cycles, with unchanged integrity and morphology. Additionally, wide substrate scopes were achieved for both of the catalytic reactions under optimized conditions. These findings highlight the potential of nitrogen-rich MOFs as sustainable catalysts for CO conversion and valuable chemical synthesis.
二氧化碳（CO₂）是一种主要的温室气体，会带来严重的环境和健康风险。将CO₂转化为有价值的化学品或燃料为减少对化石燃料的依赖提供了一种可持续的解决方案。金属有机框架（MOFs）由于其孔隙率、富氮配体和双路易斯酸碱活性位点，在CO₂环加成反应中是高效催化剂，可提高催化效率并实现CO₂的高效利用。因此，我们设计了一种具有富氮配体的稳定微孔MOF。这种活化的MOF（）表现出卓越的稳定性和高比表面积，能有效地将CO₂分子吸附到其孔中。在温和条件下，使用（）能有效地将CO₂和环氧化物转化为环状碳酸酯，表现出优异的催化性能。即使在第四个循环后，催化剂（）仍表现出出色的催化活性，效率损失极小。此外，还以（）为催化剂，在甲苯中吲哚与β-硝基苯乙烯的傅克烷基化反应中测试了（）的催化性能。该固体在四个循环中保持其活性，完整性和形态不变。此外，在优化条件下，两种催化反应都实现了广泛的底物范围。这些发现突出了富氮MOFs作为CO₂转化和有价值化学合成的可持续催化剂的潜力。
