Cyclic Carbonate Formation from Epoxides and CO(2) Catalyzed by Sustainable Alkali Halide-Glycol Complexes: A DFT Study to Elucidate Reaction Mechanism and Catalytic Activity

可持续碱金属卤化物-乙二醇络合物催化环氧化物与CO₂生成环状碳酸酯:基于DFT计算的反应机理及催化活性研究

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Abstract

We provide a comprehensive DFT investigation of the mechanistic details of CO(2) fixation into styrene oxide to form styrene carbonate, catalyzed by potassium iodide-tetraethylene glycol complex. A detailed view on the intermediate steps of the overall reaction clarifies the role of hydroxyl substances as co-catalysts for the alkali halide-catalyzed cycloaddition. The increase of iodide nucleophilicity in presence of tetraethylene glycol is examined and rationalized by NBO and Hirshfeld charge analysis, and bond distances. We explore how different alkali metal salts and glycols affect the catalytic performance. Our results provide important hints on the synthesis of cyclic carbonates from CO(2) and epoxides promoted by alkali halides and glycol complexes, allowing the development of more efficient catalysts.

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