A Metal–Organic Framework Catalyst Facilitating Transformation of CO2 and Styrene Oxide into Styrene Carbonate and Friedel–Crafts Alkylation

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Priti Bera, Kalimuthu Abirami Sundari, Veerappan Karthik, Pritam Das, Pil-Ryung Cha, Amarajothi Dhakshinamoorthy* and Shyam Biswas*, 
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Abstract

Carbon dioxide (CO2) is a major greenhouse gas that poses serious environmental and health risks. Converting CO2 into valuable chemicals or fuels offers a sustainable solution to reducing fossil fuel dependence. Metal–organic frameworks (MOFs) are efficient catalysts in CO2 cycloaddition due to their porosity, nitrogen-rich ligands, and dual Lewis acid–base active sites, enhancing catalytic efficiency and enabling efficient CO2 utilization. Therefore, we designed a stable microporous MOF with a nitrogen-rich ligand. This activated MOF (1′) demonstrates exceptional stability and high surface area, which is effective for the adsorption of CO2 molecules into its pore. The use of 1′ efficiently converts CO2 and epoxides into cyclic carbonates under moderate conditions, exhibiting an excellent catalytic performance. Catalyst 1′ showed outstanding catalytic activity even after a fourth cycle with a minimal loss of its efficiency. Furthermore, the catalytic performance of 1′ was also tested in the Friedel–Crafts alkylation of indole with β-nitrostyrene in toluene using 1′ 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 CO2 conversion and valuable chemical synthesis.

Abstract Image

一种促进二氧化碳和氧化苯乙烯转化为碳酸苯乙烯和Friedel-Crafts烷基化的金属-有机骨架催化剂。
二氧化碳(CO2)是造成严重环境和健康风险的主要温室气体。将二氧化碳转化为有价值的化学物质或燃料为减少对化石燃料的依赖提供了一个可持续的解决方案。金属有机骨架(MOFs)由于其多孔性、富氮配体和双路易斯酸碱活性位点,提高了催化效率,实现了CO2的高效利用,是CO2环加成的高效催化剂。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(1’)具有优异的稳定性和高的比表面积,可以有效地将CO2分子吸附到其孔中。在中等条件下,使用1′能有效地将CO2和环氧化物转化为环状碳酸盐,表现出优异的催化性能。催化剂1’即使在第四次循环后也表现出优异的催化活性,其效率损失最小。此外,还测试了1′作为催化剂在甲苯中吲哚与β-硝基苯乙烯的Friedel-Crafts烷基化反应中的催化性能。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,两种催化反应的底物范围都很广。这些发现突出了富氮mof作为CO2转化和有价值的化学合成的可持续催化剂的潜力。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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