Abstract:
Porous organic polymers (POPs) with high porosity and tunable functionalities have been widely studied for use in gas separation, catalysis, energy conversion and energy storage. However, the high cost of organic monomers, and the use of toxic solvents and high temperatures during synthesis pose obstacles for large-scale production. Herein, we report the synthesis of imine and aminal-linked POPs using inexpensive diamine and dialdehyde monomers in green solvents. Theoretical calculations and control experiments show that using meta-diamines is crucial for forming aminal linkages and branching porous networks from [2+2] polycondensation reactions. The method demonstrates good generality in that 6 POPs were successfully synthesized from different monomers. Additionally, we scaled up the synthesis in ethanol at room temperature, resulting in the production of POPs in sub-kilogram quantities at a relatively low cost. Proof-of-concept studies demonstrate that the POPs can be used as high-performance sorbents for CO2 separation and as porous substrates for efficient heterogeneous catalysis. This method provides an environmentally friendly and cost-effective approach for large-scale synthesis of various POPs.
摘要:
具有高孔隙率和可调功能的多孔有机聚合物(POPs)已被广泛研究用于气体分离,催化作用,能量转换和能量储存。然而,有机单体的高成本,并且在合成过程中使用有毒溶剂和高温对大规模生产构成障碍。在这里,我们报道了在绿色溶剂中使用廉价的二胺和二醛单体合成亚胺和缩醛胺连接的POPs。理论计算和对照实验表明,使用间二胺对于从[22]缩聚反应形成胺基连接和支化多孔网络至关重要。该方法具有良好的通用性,因为从不同的单体成功合成了6种POPs。此外,我们在室温下在乙醇中放大合成,导致以相对较低的成本生产亚千克数量的持久性有机污染物。概念验证研究表明,POPs可用作CO2分离的高性能吸附剂,也可用作有效多相催化的多孔基质。该方法为大规模合成各种POPs提供了一种环境友好且经济有效的方法。