自支撑多孔有机胺聚合物的设计、合成及生长机制研究

Much attention has been paid to the global climate change and ecological environment deterioration that result from greenhouse effect. The development of efficient, low-cost materials for CO2 capture has thus become quite urgent. Traditionally, adsorbents were prepared by introducing active components such as organic amine to porous supports. However, the supports cannot adsorb any CO2 at all, which limits the overall adsorption capacity of adsorbents. In addition, the supports have to be heated simultaneously in the process of regeneration, and the cost is therefore raised due to the consumption of energy. In this project, a new strategy will be developed to construct support-free porous polyamines. The assembly of two monomers under mild conditions will be realized via alkylation of amine, leading to the formation of multidimensional polymers decorated with amines. The resultant polyamines are supposed to show high density of active sites, high stability, and moderate adsorption strength. The accurate control of structure and performance of polymers will be realized by rational design and optimization of monomers. By clarifying the mechanism for polymer synthesis, it is expected to provide guidance for the development of novel functional materials derived from support-free porous polyamines. The application of new generation adsorbents may break the limitation of conventional materials, which results in an efficient, low-cost process for the removal of CO2, and promotes the upgrade of related industries including carbon capture in power plants and natural gas purification.

温室效应引起的全球气候变化和生态环境恶化问题备受关注，开发高效、低成本的CO2捕获材料已迫在眉睫。传统的吸附材料一般是将有机胺等活性组分引入到多孔载体中。然而，载体本身并不具备吸附能力，这在很大程度上限制了吸附剂中活性位密度的提高；另外，载体在再生过程中需要同时被加热而消耗能量，这无疑提高了过程的成本。项目针对传统吸附剂存在的问题，提出构筑自支撑多孔有机胺聚合物的新思路。通过胺的烷基化反应实现温和条件下两种单体的组装，形成镶嵌氨基的多维聚合物网络。所研制的吸附剂同时具备高的活性位密度、强的稳定性和适中的吸附强度。拟通过单体结构的理性设计和优化，实现目标材料结构和性能的精确控制；揭示聚合物的生长机制，为基于自支撑多孔有机胺聚合物的新型功能材料的开发提供指导。通过新一代吸附材料的运用，有望打破传统吸附剂的限制，实现CO2的高效、低成本捕获，推动发电厂脱碳和天然气净化等相关行业的技术升级。

二氧化碳吸附分离是实现碳捕集与碳中和的重要环节和手段，含氮多孔有机聚合物及其衍生的氮掺杂多孔碳可作为高效的二氧化碳吸附剂。本项目首先选取、合成并考察了不同的卤代芳烃和含氮有机单体组合对聚合反应模式以及聚合物结构的影响，然后考察不同的聚合物制备方法与含氮基团引入方式对于含氮多孔有机聚合物合成效果以及组织功能的影响，以及后续产生的氮掺杂多孔碳的组织结构以及吸附分离性能的差异。最后在实验研究的基础上，本项目通过量子化学计算推导出多孔有机聚合物的构筑模式和原理，及其衍生多孔碳的产生机制，并结合其对二氧化碳等吸附质吸附分离的计算模拟，推导不同的氮掺杂位点和吸附剂组织结构引起吸附性能差异的本质，并给出明确的构效关系。

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