Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO2 Fixing

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• 作者：Balaka Barkakaty ; Katie L. Browning ; Bobby Sumpter ; David Uhrig ; Ivana Karpisova ; Kevin W. Harman ; Ilia Ivanov ; Dale K. Hensley ; Jamie M. Messman ; S. Michael Kilbey II ; Bradley S. Lokitz
• 刊名：Macromolecules
• 出版年：2016
• 出版时间：March 8, 2016
• 年：2016
• 卷：49
• 期：5
• 页码：1523-1531
• 全文大小：443K
• ISSN：1520-5835

文摘

Development of novel polymeric materials capable of efficient CO<sub>2sub> capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO<sub>2sub>-responsive polymer through postpolymerization modification of poly(2-vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine)benzyl alcohol (PBA) without any byproduct formation. FTIR and TGA experiments show the new PBA-functionalized polymer powder can reversibly capture CO<sub>2sub> at room temperature and under atmospheric pressure. CO<sub>2sub> capture was selective, showing a high fixing efficiency even with a mixed gas system (20% CO<sub>2sub>, 80% N<sub>2sub>) similar to flue gas. CO<sub>2sub> release occurred at room temperature, and release profiles were investigated as a function of temperature. Density functional theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO<sub>2sub> binding sites in the PBA-functionalized polymer resulting in a two-step CO<sub>2sub> release at room temperature. The ease of material preparation, high fixing efficiency, and robust release characteristics suggest that postpolymerization modification may be a useful route to designing new materials for CO<sub>2sub> capture.