We review the literature on the use of computational methods to study the reactions between carbon dioxide and aqueous organic amines used to capture CO₂ prior to storage, reuse, or sequestration. The focus is largely on the use of high level quantum chemical methods to study these reactions, although the review also summarizes research employing hybrid quantum mechanics/molecular mechanics methods and molecular dynamics. We critically review the effects of basis set size, quantum chemical method, solvent models, and other factors on the accuracy of calculations to provide guidance on the most appropriate methods, the expected performance, method limitations, and future needs and trends. The review also discusses experimental studies of amine-CO₂ equilibria, kinetics, measurement and prediction of amine pK_a values, and degradation reactions of aqueous organic amines. Computational simulations of carbon capture reaction mechanisms are also comprehensively described, and the relative merits of the zwitterion, termolecular, carbamic acid, and bicarbonate mechanisms are discussed in the context of computational and experimental studies. Computational methods will become an increasingly valuable and complementary adjunct to experiments for understanding mechanisms of amine-CO₂ reactions and in the design of more efficient carbon capture agents with acceptable cost and toxicities.

中文翻译：

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胺类捕集CO _2的计算建模与仿真

我们回顾了有关使用计算方法研究在存储，再利用或封存之前用于捕获CO _2的二氧化碳与水性有机胺之间反应的文献。尽管本综述还总结了采用混合量子力学/分子力学方法和分子动力学的研究，但重点主要在于使用高级量子化学方法来研究这些反应。我们严格审查了基集大小，量子化学方法，溶剂模型和其他因素对计算准确性的影响，以为最合适的方法，预期的性能，方法的局限性以及未来的需求和趋势提供指导。该评论还讨论了胺-CO _2的实验研究胺p K _a值的平衡，动力学，测量和预测，以及有机胺水溶液的降解反应。还全面描述了碳捕获反应机理的计算模拟，并在计算和实验研究的背景下讨论了两性离子，分子，氨基甲酸和碳酸氢根机理的相对优点。计算方法将成为用于了解胺-CO ₂反应机理和设计具有可接受的成本和毒性的更有效的碳捕获剂的实验的一种越来越有价值的补充方法。