论文标题
集体现象如何影响不同媒体的二氧化碳反应性和物种形成
How collective phenomena impact CO2 reactivity and speciation in different media
论文作者
论文摘要
由于其在温室效应和环境管理中的作用，CO2在近年来引起了很大的关注。尽管已经对其与水的反应进行了广泛的研究，但在超临界二氧化碳相的反应性方面不能说相同，在这种反应性的情况下，共轭酸/碱基平衡通过不同的机制和激活屏障进行。尽管CO2 + H2O反应的明显简单性，但不同环境的集体效应对自由能曲线的影响很大。增强的采样技术和量身定制的集体变量提供了焓和熵驱动器的详细图片，强调了气体，水和超临界二氧化碳中碳酸形成机制的差异。
CO2 has attracted considerable attention in the recent years due to its role in the greenhouse effect and environmental management. While its reaction with water has been studied extensively, the same cannot be said for reactivity in supercritical CO2 phase, where the conjugate acid/base equilibria proceed through different mechanisms and activation barriers. In spite of the apparent simplicity of the CO2 + H2O reaction, the collective effect of different environments has drastic influence on the free energy profile. Enhanced sampling techniques and well-tailored collective variables provide a detailed picture of the enthalpic and entropic drivers underscoring the differences in the formation mechanism of carbonic acid in the gas, aqueous and supercritical CO2 phases.
