期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 10, 期 10, 页码 5540-5549出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta10312a
关键词
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资金
- National Natural Science Foundation of China [21603089]
- Natural Science Foundation of Jiangsu Province [BK20160209]
- Natural Science Foundation of Jiangsu Higher Education Institutions of China [16KJB150014]
- Postgraduate Research & Practice Innovation Program of Jiangsu Province [KYCX21_2570]
- Top-notch Academic Programs Project of Jiangsu Higher Education Institutions (TAPP)
This work presents a facile strategy to fabricate a new class of viologen-linked ionic polyacetylenes (VIPAs) through catalyst-free and initiator-free polymerization. The highly cross-linked VIPAs show excellent catalytic activity for the conversion of CO2 with various epoxides into cyclic carbonates. The reaction temperature has a significant influence on the synthesis of VIPAs, achieving the transformation from soluble oligomers to insoluble polymers.
In this work, we reported a facile catalyst-free and initiator-free strategy to fabricate a new class of viologen-linked ionic polyacetylenes (denoted as VIPAs) that can achieve simultaneous ionization and polymerization in one-pot and one-step. To our surprise, the ionic polymers VIPA-X (X = Br or Cl) were directly synthesized by quaternization-induced in situ polymerization from commercially available 4,4 '-bipyridine with propargyl bromide or propargyl chloride. It was found that reaction temperatures have a remarkable influence on the synthesis of VIPAs, achieving the transformation from soluble oligomers to insoluble highly cross-linked polymers by adjusting the temperatures from 30 degrees C to 100 degrees C. At a higher temperature of 100 degrees C, the obtained highly cross-linked ionic polymers VIPA-Br and VIPA-Cl were insoluble in both hot water and even dimethyl sulfoxide (DMSO). By virtue of abundant halogen anions and the absorbed H-bonded water, both VIPA-Br and VIPA-Cl were employed as efficient heterogeneous catalysts for the conversion of CO2 with various epoxides into cyclic carbonates at atmospheric pressure and low temperatures. In particular, the catalytic activities of VIPA-Br for the conversion of various epoxides are much better than those of VIPA-Cl at low temperatures, which should be attributed to the higher nucleophilicity and better leaving ability of the Br- anion than those of the Cl- anion. The present work affords a succinct catalyst-free strategy to construct more task-specific ionic polyacetylenes by quaternization-induced polymerization of multi-N-heterocycle monomers and propargyl halides towards diverse applications.
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