阐明 CALF-20 中 H2O 和 CO2 的竞争吸附：增强碳捕获金属有机框架的新见解,ACS Applied Materials & Interfaces

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阐明 CALF-20 中 H2O 和 CO2 的竞争吸附：增强碳捕获金属有机框架的新见解
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-10-05 , DOI: 10.1021/acsami.3c11092
Ching-Hwa Ho ₁ , Francesco Paesani _{1,

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Affiliation

鉴于对高效碳捕获解决方案的迫切需求，我们的研究研究了CALF-20（一种高度可扩展且稳定的金属）中水 (H ₂ O) 和二氧化碳 (CO ₂ ) 的同时吸附与相对湿度的关系——有机框架（MOF）。先进的计算机模拟表明，由于它们与框架的相互作用相似，H ₂ O 和 CO ₂分子竞争相同的结合位点，占据 CALF-20 孔内相似的空隙区域。这种竞争导致 H ₂ O 和 CO ₂分子不同的热力学和动力学行为，具体取决于是否存在一种或两种客体物种。_{值得注意的是，CO 2}分子的存在迫使H ₂ O分子在较小的区域内形成更多连接的氢键网络，减缓水的重新取向动力学并降低水的熵。相反，水的存在加速了CO ₂分子的重新定向，降低了CO ₂熵，并且由于更强的水介导的相互作用而增加了CO ₂在框架内被吸附的倾向。由于对相同空隙空间的竞争，当存在其他客体物种的分子时， H ₂ O和CO _{2分子都表现出较慢的扩散。}这些发现为增强专为碳捕获应用而设计的 MOF的 H ₂ O 和 CO ₂差异亲和力提供了有价值的策略和见解。

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Elucidating the Competitive Adsorption of H2O and CO2 in CALF-20: New Insights for Enhanced Carbon Capture Metal–Organic Frameworks

In light of the pressing need for efficient carbon capture solutions, our study investigates the simultaneous adsorption of water (H₂O) and carbon dioxide (CO₂) as a function of relative humidity in CALF-20, a highly scalable and stable metal–organic framework (MOF). Advanced computer simulations reveal that due to their similar interactions with the framework, H₂O and CO₂ molecules compete for the same binding sites, occupying similar void regions within the CALF-20 pores. This competition results in distinct thermodynamic and dynamical behaviors of H₂O and CO₂ molecules, depending on whether one or both guest species are present. Notably, the presence of CO₂ molecules forces the H₂O molecules to form more connected hydrogen-bond networks within smaller regions, slowing water reorientation dynamics and decreasing water entropy. Conversely, the presence of water speeds up the reorientation of CO₂ molecules, decreases the CO₂ entropy, and increases the propensity for CO₂ to be adsorbed within the framework due to stronger water-mediated interactions. Due to the competition for the same void spaces, both H₂O and CO₂ molecules exhibit slower diffusion when molecules of the other guest species are present. These findings offer valuable strategies and insights into enhancing the differential affinity of H₂O and CO₂ for MOFs specifically designed for carbon capture applications.

更新日期：2023-10-05

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