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Substoichiometric 3D Covalent Organic Frameworks Based on Hexagonal Linkers
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-06-30 , DOI: 10.1021/jacs.1c03739 Liangjun Chen 1 , Chengtao Gong 1 , Xiaokang Wang 2 , Fangna Dai 2 , Mingchu Huang 1 , Xiaowei Wu 3, 4 , Can-Zhong Lu 3, 4, 5 , Yongwu Peng 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-06-30 , DOI: 10.1021/jacs.1c03739 Liangjun Chen 1 , Chengtao Gong 1 , Xiaokang Wang 2 , Fangna Dai 2 , Mingchu Huang 1 , Xiaowei Wu 3, 4 , Can-Zhong Lu 3, 4, 5 , Yongwu Peng 1
Affiliation
Covalent organic frameworks (COFs), a fast-growing field in crystalline porous materials, have achieved tremendous success in structure development and application exploration over the past decade. The vast majority of COFs reported to date are designed according to the basic concept of reticular chemistry, which is rooted in the idea that building blocks are fully connected within the frameworks. We demonstrate here that sub-stoichiometric construction of 2D/3D COFs can be accomplished by the condensation of a hexagonal linker with 4-connected building units. It is worth noting that the partially connected frameworks were successfully reticulated for 3D COFs for the first time, representing the highest BET surface area among imine-linked 3D COFs to data. The unreacted benzaldehydes in COF frameworks can enhance C2H2 and CO2 adsorption capacity and selectivities between C2H2/CH4 and C2H2/CO2 for sub-stoichiometric 2D COFs, while the reserved benzaldehydes control the interpenetrated architectures for the 3D case, achieving a rare non-interpenetrated pts topology for 3D COFs. This work not only paves a new avenue to build new COFs and endows residual function groups with further applications but also prompts redetermination of reticular frameworks in highly connected and symmetrical COFs.
中文翻译:
基于六边形接头的亚化学计量 3D 共价有机框架
共价有机骨架(COFs)是结晶多孔材料中一个快速发展的领域,在过去十年中在结构开发和应用探索方面取得了巨大成功。迄今为止报道的绝大多数 COF 都是根据网状化学的基本概念设计的,其植根于构建模块在框架内完全连接的想法。我们在这里证明了 2D/3D COF 的亚化学计量构造可以通过六边形接头与 4 个连接的构建单元的缩合来实现。值得注意的是,部分连接的框架首次成功网状化用于 3D COF,代表了亚胺连接的 3D COF 数据中最高的 BET 表面积。COF骨架中未反应的苯甲醛可以增强C 2H 2和CO 2吸附容量和C 2 H 2 /CH 4和C 2 H 2 /CO 2 之间对于亚化学计量2D COFs的选择性,而保留的苯甲醛控制3D情况下的互穿结构,实现了罕见的非-用于 3D COF 的互穿 pts 拓扑。这项工作不仅为构建新的 COF 铺平了新的途径,并赋予了残差函数群进一步的应用,而且还促使重新确定高度连接和对称的 COF 中的网状框架。
更新日期:2021-07-14
中文翻译:
基于六边形接头的亚化学计量 3D 共价有机框架
共价有机骨架(COFs)是结晶多孔材料中一个快速发展的领域,在过去十年中在结构开发和应用探索方面取得了巨大成功。迄今为止报道的绝大多数 COF 都是根据网状化学的基本概念设计的,其植根于构建模块在框架内完全连接的想法。我们在这里证明了 2D/3D COF 的亚化学计量构造可以通过六边形接头与 4 个连接的构建单元的缩合来实现。值得注意的是,部分连接的框架首次成功网状化用于 3D COF,代表了亚胺连接的 3D COF 数据中最高的 BET 表面积。COF骨架中未反应的苯甲醛可以增强C 2H 2和CO 2吸附容量和C 2 H 2 /CH 4和C 2 H 2 /CO 2 之间对于亚化学计量2D COFs的选择性,而保留的苯甲醛控制3D情况下的互穿结构,实现了罕见的非-用于 3D COF 的互穿 pts 拓扑。这项工作不仅为构建新的 COF 铺平了新的途径,并赋予了残差函数群进一步的应用,而且还促使重新确定高度连接和对称的 COF 中的网状框架。