1. Implanting multi-functional ionic liquids into MOF nodes for boosting CO2 cycloaddition under solventless and cocatalyst-free conditions.
- Author
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Chen, Yan, Li, Fangfang, Liu, Laiyao, and Zhou, Ying-Hua
- Subjects
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IONIC liquids , *HETEROGENEOUS catalysts , *RING formation (Chemistry) , *LEWIS acidity , *CARBON offsetting , *CARBON dioxide , *CARBON dioxide adsorption - Abstract
• MIL-101(Cr) nodes were tethered by ionic liquids bearing hydrogen-bond donor. • MIL-101(Cr) derivative as catalyst boosted the epoxide cycloaddition with CO 2. • The heterogeneous catalyst containing carboxyl displayed superior activity. • The catalyst exhibited the great durability and recyclability. It is critical to design an effective catalyst for CO 2 conversion into cyclocarbonate to achieve the carbon neutrality. Herein, MIL-101(Cr) tethered by hydrogen bond donors (HBD)-containing ionic liquids (denoted as MIL-101-ILs(R), R = OH, NH 2 , and COOH) were synthesized through the implantation of 4,4′-bipyridine into MOF nodes via the post-synthetic modification, followed by the decoration with bromoalkanes including bromoethanol, bromoethylamine, and bromoacetic acid. Their catalytic performance were evaluated by the epoxide cycloaddition reaction under 1.0 MPa CO 2 and 80 ℃ for 6 h in the absence of solvent and cocatalyst. Compared to MIL-101-ILs without HBD, MIL-101-ILs(OH) and MIL-101-ILs(NH 2) demonstrated the more chloropropene carbonate (CPC) yield of 88 % and 83 %, respectively. Notably, MIL-101-ILs(COOH) exhibited an uppermost activity with a CPC yield of 96 %, attributed to the cooperativity of Lewis acidity originating from Cr 3 O clusters, hydrogen-bond interaction afforded by carboxyl groups, and the strong nucleophilicity offered by Br- ions of ILs. Moreover, MIL-101-ILs(COOH) presented excellent recyclability. A potential catalytic mechanism for epoxide cycloaddition with CO 2 into cyclic carbonate has been proposed. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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