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Ordered Macro–Microporous Single Crystals of Covalent Organic Frameworks with Efficient Sorption of Iodine
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-01-20 , DOI: 10.1021/jacs.2c12284
Tong Liu 1 , Yi Zhao 1 , Min Song 1 , Xinghan Pang 1 , Xiaofei Shi 1 , Jingjing Jia 1 , Lifeng Chi 1 , Guang Lu 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-01-20 , DOI: 10.1021/jacs.2c12284
Tong Liu 1 , Yi Zhao 1 , Min Song 1 , Xinghan Pang 1 , Xiaofei Shi 1 , Jingjing Jia 1 , Lifeng Chi 1 , Guang Lu 1
Affiliation
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Fashioning microporous covalent organic frameworks (COFs) into single crystals with ordered macropores allows for an effective reduction of the mass transfer resistance and the maximum preservation of their intrinsic properties but remains unexplored. Here, we report the first synthesis of three-dimensional (3D) ordered macroporous single crystals of the imine-linked 3D microporous COFs (COF-300 and COF-303) via a template-assisted modulated strategy. In this strategy, COFs crystallized within the sacrificial colloidal crystal template, assembled from monodisperse polystyrene microspheres, and underwent an aniline-modulated amorphous-to-crystalline transformation to form large single crystals with 3D interconnected macropores. The effects of the introduced macroporous structure on the sorption performances of COF-300 single crystals were further probed by iodine. Our results indicate that iodine adsorption occurred in micropores of COF-300 but not in the introduced macropores. Accordingly, the iodine adsorption capacity of COF single crystals was governed by their micropore accessibility. The relatively long diffusion path in the non-macroporous COF-300 single crystals resulted in a limited micropore accessibility (48.4%) and thus a low capacity in iodine adsorption (1.48 g·g–1). The introduction of 3D ordered macropores can greatly shorten the microporous diffusion path in COF-300 single crystals and thus render all their micropores fully accessible in iodine adsorption with a capacity (3.15 g·g–1) that coincides well with the theoretical one.
中文翻译：
高效吸附碘的共价有机骨架有序大微孔单晶
将微孔共价有机框架 (COF) 制成具有有序大孔的单晶，可以有效降低传质阻力并最大程度地保留其固有特性，但仍未得到探索。在这里，我们报告了通过模板辅助调制策略首次合成亚胺连接的 3D 微孔 COF（COF-300 和 COF-303）的三维 (3D) 有序大孔单晶。在该策略中，COF 在牺牲胶体晶体模板内结晶，由单分散聚苯乙烯微球组装而成，并经历苯胺调制的无定形到结晶转变，形成具有 3D 互连大孔的大单晶。通过碘进一步探究引入大孔结构对COF-300单晶吸附性能的影响。我们的结果表明，碘吸附发生在 COF-300 的微孔中，而不是在引入的大孔中。因此，COF单晶的碘吸附能力受其微孔可达性的控制。非大孔 COF-300 单晶中相对较长的扩散路径导致微孔可及性有限（48.4%），因此碘吸附容量较低（1.48 g·g–1）。3D有序大孔的引入可以大大缩短COF-300单晶中的微孔扩散路径，从而使其所有微孔在碘吸附中完全可用，其容量（3.15 g·g –1）与理论值非常吻合。
更新日期：2023-01-20
中文翻译：
高效吸附碘的共价有机骨架有序大微孔单晶
将微孔共价有机框架 (COF) 制成具有有序大孔的单晶，可以有效降低传质阻力并最大程度地保留其固有特性，但仍未得到探索。在这里，我们报告了通过模板辅助调制策略首次合成亚胺连接的 3D 微孔 COF（COF-300 和 COF-303）的三维 (3D) 有序大孔单晶。在该策略中，COF 在牺牲胶体晶体模板内结晶，由单分散聚苯乙烯微球组装而成，并经历苯胺调制的无定形到结晶转变，形成具有 3D 互连大孔的大单晶。通过碘进一步探究引入大孔结构对COF-300单晶吸附性能的影响。我们的结果表明，碘吸附发生在 COF-300 的微孔中，而不是在引入的大孔中。因此，COF单晶的碘吸附能力受其微孔可达性的控制。非大孔 COF-300 单晶中相对较长的扩散路径导致微孔可及性有限（48.4%），因此碘吸附容量较低（1.48 g·g–1）。3D有序大孔的引入可以大大缩短COF-300单晶中的微孔扩散路径，从而使其所有微孔在碘吸附中完全可用，其容量（3.15 g·g –1）与理论值非常吻合。
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