近日，英国利物浦大学Cooper, Andrew I.团队研究了面向湿气CO₂捕集的形状选择有机大环自下而上的计算设计。该项研究成果发表在2025年7月22日出版的《自然-化学》杂志上。

捕获以多孔固体为主题的二氧化碳排放具有挑战性，因为在大多数材料中，极性水分子比非极性二氧化碳分子结合更强。这对烟气捕集和直接空气捕集都是一个挑战。

研究组开发了一个自下而上的计算筛选工作流程来计算27,446个不同的分子片段与CO₂和水的结合能。大多数分子倾向于与水结合，但弯曲的、夹状的芳香分子表现出期望的反向选择性的潜力。这表明具有特定形状的芳香族大环可以促进与CO₂的多重弱π -π相互作用，而不是与水的强而少的偶极子-π相互作用。

根据计算结果，研究组合成了两种具有三角形和正方形几何形状的水稳定和酸稳定分子“棱镜”。实验证实，这些棱镜的二氧化碳捕获能力不受高相对湿度的影响，超过了基准商业多孔材料的性能。

附：英文原文

Title: Bottom-up computational design of shape-selective organic macrocycles for humid CO2 capture

Author: Liu, Tao, Qu, Hang, Harding, Sam D., Borne, Isaiah, Chen, Linjiang, Ward, John W., Weston, Simon C., Cooper, Andrew I.

Issue&Volume: 2025-07-22

Abstract: The capture of CO2 emissions using porous solids is challenging because polar water molecules bind more strongly in most materials than non-polar CO2 molecules. This is a challenge for both flue gas capture and for direct air capture alike. Here we develop a bottom-up computational screening workflow to calculate the binding energy of 27,446 diverse molecular fragments with both CO2 and water. Most molecules favour water binding, but bent, clip-like aromatic molecules exhibit potential for the desired reverse selectivity. This suggests that aromatic macrocycles with specific shapes can promote multiple weak π–π interactions with CO2 that surpass stronger but less numerous dipole–π interactions with water. We synthesize two water- and acid-stable molecular prisms with triangular and square geometries, as suggested by computation. Experiments confirm that the CO2 capture capacity of these prisms is unaffected by high relative humidity, surpassing the performance of benchmark commercial porous materials.

DOI: 10.1038/s41557-025-01873-1

Source: https://www.nature.com/articles/s41557-025-01873-1