A dual-ionic hyper-crosslinked polymer for efficient CO2 fixation and conversion
CHEMICAL ENGINEERING JOURNAL(2024)
摘要
It is of great significance for reducing carbon emissions and protecting the environment to convert carbon dioxide (CO2) into high-value chemicals. The cycloaddition of CO2 with epoxides to prepare cyclic carbonates is a very attractive and potential approach. However, due to the inherent chemical inertness of CO2, the development of highly efficient, metal-free, solvent-free, and co-catalyst-free heterogeneous catalysts is crucial. Herein, a dualionic system hyper-cross-linked polymer (HIP-COOH-TMG) was synthesized by a post-synthetic strategy. HIPCOOH-TMG with multiple active sites was characterized by FT-IR, XPS and other characterizations. HIPCOOH-TMG exhibited the excellent catalytic activity than HIP-COOH for the CO2 cycloaddition, the yield and selectivity of chloropropene carbonate (CC) reached 99 % within 8 h at 110 degrees C under 1 MPa CO2 pressure. In addition, HIP-COOH-TMG is easily separated from the product, has good recyclability and structural stability, and exhibits high activity towards a series of epoxides. Finally, density functional theory (DFT) calculations reveal the synergistic catalytic mechanism of hydrogen bond donors (HBDs) groups 1/4 NH2+ sites and N sites activation of HIP-COOH-TMG, providing a reference for the design of metal-free, co-catalyst-free, and solventfree heterogeneous catalysts.
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关键词
CO2 cycloaddition,Hydrogen bond donors,Hyper-cross-linked polymers,Dual ionic liquids,TMG
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