具有复杂分层空间配置的上层结构比单个分层结构具有更宽的结构深度和更广泛的应用前景。然而,目前的制备方法受到繁琐的步骤和苛刻的条件的极大限制。这里,我们呈现,第一次,一种简洁有效的热响应动态合成策略,用于在可溶性共价有机网络(SCONS)内制备多维复杂的超结构,具有从0D中空超颗粒到2D薄膜的可调形态。机理研究揭示了SCONS的热响应动态“裂解-重塑”特性,基于[2.2]对环烷独特的双层结构合成,和温度控制促进了从可逆溶解度到重组和构建上部结构的过程。具体来说,在这个过程中,油水乳液两相界面可以通过液滴喷射产生,导致制备0D中空超颗粒和其他碗状复杂超结构,产量高。此外,通过调节外源溶剂的挥发性和溶解度,基于气液界面制备了无缺陷的2D薄膜。扩展的实验进一步证实了所提出的动态“分裂-重塑”策略的普遍性和可扩展性。客体碘富集机理的研究突出了超结构产物相对于单层材料的优越的动力学传质性能。这项研究不仅为上层建筑的建设提供了一条创新的捷径,也是体现上层建筑优势及其广泛应用的科学依据。本文受版权保护。保留所有权利。
Superstructures with complex hierarchical spatial configurations exhibit broader structural depth than single hierarchical structures and the associated broader application prospects. However, current preparation methods are greatly constrained by cumbersome steps and harsh conditions. Here, for the first time, a concise and efficient thermally responsive dynamic synthesis strategy for the preparation of multidimensional complex
superstructures within soluble covalent organic networks (SCONs) with tunable morphology from 0D hollow supraparticles to 2D films is presented. Mechanism study reveals the thermally responsive dynamic \"cleavage-remodeling\" characteristics of SCONs, synthesized based on the unique bilayer structure of (2.2)paracyclophane, and the temperature control facilitates the process from reversible solubility to reorganization and construction of
superstructures. Specifically, during the process, the oil-water-emulsion two-phase interface can be generated through droplet jetting, leading to the preparation of 0D hollow supraparticles and other bowl-like complex
superstructures with high yield. Additionally, by modulating the volatility and solubility of exogenous solvents, defect-free 2D films are prepared relying on an air-liquid interface. Expanded experiments further confirm the generalizability and scalability of the proposed dynamic \"cleavage-remodeling\" strategy. Research on the enrichment mechanism of guest iodine highlights the superior kinetic mass transfer performance of superstructural products compared to single-hierarchical materials.