Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 23, Issue 3, Pages 2005-2014Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cp06041k
Keywords
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Funding
- Innovation Academy for Green Manufacture, Chinese Academy of Sciences [IAGM-2019-A01]
- Transformational Technologies for Clean Energy and Demonstration'', Strategic Priority Research Program of the Chinese Academy of Sciences [XDA 21030500]
- National Natural Science Foundation of China [21890763, 21908226]
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The study successfully synthesized a heterogeneous catalyst with high efficiency and recyclability by introducing hydrogen bond donor (HBD) groups into poly(ionic liquid)s, enabling the conversion of CO2 into high value-added products. Experimental results demonstrated that HBD-functionalized poly(ionic liquid)s exhibited excellent catalytic performance and recyclability, suggesting a promising approach for green technology utilizing poly(ionic liquid)s.
The development of metal-free, high effective and recyclable catalysts plays a pivotal role in transforming CO2 into high value-added products such as cyclic carbonates. In this paper, we introduced the hydrogen bond donor (HBD) groups into poly(ionic liquid)s via free radical polymerization, which successfully combined the HBD and ionic liquids (ILs) into one heterogeneous catalyst. The HBD could synergistically activate epoxides with hydroxyl functionalized ionic liquids and efficiently catalyze the cycloaddition of CO2 into cyclic carbonates. The yield of propylene carbonate (PC) reached 94% (at 105 degrees C, 2 MPa CO2, 3 h), which far exceeded poly(ionic liquid)s without HBDs functionalization (PC yield 72%), and even approached bulk ionic liquids (PC yield 95%). Moreover, HBD-functionalized poly(ionic liquid)s (HPILs) exhibited excellent recyclability after five runs and afforded wide substrate scope. According to the experimental results, H-1 NMR spectra and density functional theory (DFT) calculations showed 2-hydroxyethyl methacrylate (HEMA) and the hydroxyl of ILs would form strong H-bonds with epoxides contributing to the ring-opening process of epoxides, and a possible HBD and nucleophilic anion synergistically catalytic mechanism was proposed. The method herein paved a brand new way for green technology and utilization of poly(ionic liquid)s.
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