Aqueous amine solution is a promising absorbent for CO2 capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO2 for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high‐performance CO2 absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti‐degradation CO2 absorbent.

中文翻译：

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用于 CO2 捕获的叔胺的热降解：构效关系和密度泛函理论计算


胺水溶液是一种很有前途的 CO2 捕获吸收剂，但反应是不可逆的，也就是说，胺会发生降解，导致性能下降和许多操作困难。尽管对胺和 CO2 之间的吸收反应进行了大量研究，但胺降解的反应尚不完全清楚，尤其是叔胺，它是构建高性能 CO2 吸收剂的重要组成部分。考虑到叔胺的种类，本文研究了 5 种叔胺溶液在不同温度下的热稳定性，以模拟再生条件。应用密度泛函理论 （DFT） 计算来揭示降解机制。触发叔胺降解的烷基化反应被认为是限制步骤。然后将分子模拟方法扩展到 12 个叔胺，旨在进一步说明分子结构对烷基化反应的影响。这些结果为开发抗降解 CO2 吸收剂提供了基础数据和理论指导。