<br>共价有机框架的水溶胶-凝胶合成和成型,Journal of the American Chemical Society

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共价有机框架的水溶胶-凝胶合成和成型
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-12-11 , DOI: 10.1021/jacs.3c10053
Fan Hu ₁ , Zeyou Hu ₁ , Yufei Liu ₁ , Kam Chiu Tam ₂ , Rongran Liang ₃ , Qiujian Xie ₁ , Zhiwen Fan ₁ , Chunyue Pan ₁ , Juntao Tang ₁ , Guipeng Yu ₁ , Wei Zhang ₄

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共价有机骨架（COF）固有的脆弱性和不溶性严重阻碍了其实际应用的加工性。本文报道了一种水基溶胶-凝胶合成策略，用于 COF 的合成和成型，具有特定任务的应用，满足晶体材料克级生产的绿色化学原理。我们的成功方法涉及三个关键方面：水溶性单体的“前药模拟”设计、可水解键的利用以及反应动力学的操纵。该方法的通用性通过使用几种常用胺成功制备代表性高表面积二维（2D）COF 得到证明。凭借这一策略，实现了 COF 胶体分散体，并且可以配制为可加工流体、结构化薄膜和 COF 整体料。值得注意的是，与广泛使用的海绵和棉花相比，所获得的轻质（∼0.020 g cm ^–3 ）和坚固的气凝胶对多种有机溶剂表现出出色的吸附能力（超过其自身重量的57倍），并且表现出优异的隔热性能。这项工作展示了一种在水中合成和成型可加工 COF 材料的多功能策略，这将有助于开发用于先进应用的 COF 整体材料。

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Aqueous Sol–Gel Synthesis and Shaping of Covalent Organic Frameworks

The intrinsic fragility and insoluble nature of covalent organic frameworks (COFs) have strongly impeded their processability for practical applications. Herein, an aqueous-based sol–gel synthetic strategy is reported for the synthesis and shaping of COFs with task-specific applications that satisfy the principles of green chemistry for gram-scale production of crystalline materials. Our successful approach involves three pivotal aspects: the “prodrug mimic” design of water-soluble monomers, the utilization of hydrolyzable bonds, and the manipulation of reaction kinetics. The generality of the method is demonstrated by the successful preparation of representative high-surface area two-dimensional (2D) COFs with several commonly used amines. By virtue of this strategy, a COF colloidal dispersion is achieved and can be formulated into processable fluids, structured films, and COF monoliths. Remarkably, the obtained lightweight (∼0.020 g cm^–3) and robust aerogels displayed outstanding adsorption capacity (exceeding 57 times its own weight) toward a variety of organic solvents and exhibited superior thermal insulating properties compared to the widely used sponge and cotton. This work demonstrates a versatile strategy for the synthesis and shaping of processable COF materials in water that will contribute to the development of COF monoliths for advanced applications.

更新日期：2023-12-11

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