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Covalent Self-assembly in Two Dimensions: Connecting Cova-lent Organic Framework Nanospheres into Crystalline and Po-rous Thin Films
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-11-29 , DOI: 10.1021/jacs.9b10788 Himadri Sekhar Sasmal 1 , Arjun Halder 1 , Shebeeb Kunjattu H 2 , Kaushik Dey 1 , Athulya Nadol 2 , Thalasseril G Ajithkumar 2 , Prachiti Ravindra Bedadur 2 , Rahul Banerjee 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-11-29 , DOI: 10.1021/jacs.9b10788 Himadri Sekhar Sasmal 1 , Arjun Halder 1 , Shebeeb Kunjattu H 2 , Kaushik Dey 1 , Athulya Nadol 2 , Thalasseril G Ajithkumar 2 , Prachiti Ravindra Bedadur 2 , Rahul Banerjee 1
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Insolubility of the Covalent Organic Frameworks (COFs) in organic solvents is one of the major obstacles for the potential application of these extended networks such as drug delivery, sensing, optoelectronics, and semiconductor device fabri-cation. The present work proposes a unique way to make uniform, solution-processable crystalline, and porous COF nanospheres directly from the homogeneous solution of amine and aldehyde via spatial and temporal control of the nu-cleation and growth. This strategy of direct nucleation simultaneously showcases the caliber to tune the size of the COF nanospheres from 25 nm to 570 nm. We have also demonstrated the concept of mesoscale covalent self-assembly of those solution-processable COF nanospheres in the liquid-liquid interface (DCM-Water bilayer) for the very first time, transmuting them into self-standing COF thin films with long-range ordered arrangements in two dimensions. The crystalline and porous (with TpAzo showing highest SBET of 1932 m2 g-1) free-standing COF thin films could be fabricated in a wide range of thicknesses from as less as 21 nm to as high as 630 nm. Both β-Ketoenamine (TpAzo, TpDPP) and imine (TpOMeAzo, TpOMeDPP) linked COF thin films have been synthesized via mesoscale covalent self-assembly of the solu-tion-processable COF nanospheres illustrating the generality of this eloquent methodology. Further, the solution processability has been tested and utilized to cast COF thin films uniformly in the inner and outer surface of the alumina hollow fiber membrane. . The COF thin film - alumina hollow fiber membrane composites have showcased promising selective molecular separation of He and O2, He and CO2 as well as He and N2.
中文翻译：
二维共价自组装：将共价有机骨架纳米球连接成结晶和多孔薄膜
共价有机框架 (COF) 在有机溶剂中的不溶性是这些扩展网络（如药物输送、传感、光电子和半导体器件制造）潜在应用的主要障碍之一。目前的工作提出了一种独特的方法，通过对成核和生长的空间和时间控制，直接从胺和醛的均匀溶液中制备均匀、可溶液加工的结晶和多孔 COF 纳米球。这种直接成核策略同时展示了将 COF 纳米球的尺寸从 25 nm 调整到 570 nm 的能力。我们还首次在液-液界面（DCM-水双层）中展示了这些可溶液加工的 COF 纳米球的中尺度共价自组装概念，将它们转变为具有二维长程有序排列的自立式 COF 薄膜。结晶和多孔（TpAzo 显示最高 SBET 为 1932 m2 g-1）自支撑 COF 薄膜可以制造，厚度范围很广，从 21 nm 到 630 nm。β-酮烯胺 (TpAzo, TpDPP) 和亚胺 (TpOMeAzo, TpOMeDPP) 连接的 COF 薄膜都是通过可溶液加工的 COF 纳米球的中尺度共价自组装合成的，说明了这种雄辩方法的普遍性。此外，溶液加工性已被测试并用于在氧化铝中空纤维膜的内表面和外表面均匀地浇铸 COF 薄膜。. COF 薄膜-氧化铝中空纤维膜复合材料展示了对 He 和 O2 的选择性分子分离，
更新日期：2019-11-29
中文翻译：
二维共价自组装：将共价有机骨架纳米球连接成结晶和多孔薄膜
共价有机框架 (COF) 在有机溶剂中的不溶性是这些扩展网络（如药物输送、传感、光电子和半导体器件制造）潜在应用的主要障碍之一。目前的工作提出了一种独特的方法，通过对成核和生长的空间和时间控制，直接从胺和醛的均匀溶液中制备均匀、可溶液加工的结晶和多孔 COF 纳米球。这种直接成核策略同时展示了将 COF 纳米球的尺寸从 25 nm 调整到 570 nm 的能力。我们还首次在液-液界面（DCM-水双层）中展示了这些可溶液加工的 COF 纳米球的中尺度共价自组装概念，将它们转变为具有二维长程有序排列的自立式 COF 薄膜。结晶和多孔（TpAzo 显示最高 SBET 为 1932 m2 g-1）自支撑 COF 薄膜可以制造，厚度范围很广，从 21 nm 到 630 nm。β-酮烯胺 (TpAzo, TpDPP) 和亚胺 (TpOMeAzo, TpOMeDPP) 连接的 COF 薄膜都是通过可溶液加工的 COF 纳米球的中尺度共价自组装合成的，说明了这种雄辩方法的普遍性。此外，溶液加工性已被测试并用于在氧化铝中空纤维膜的内表面和外表面均匀地浇铸 COF 薄膜。. COF 薄膜-氧化铝中空纤维膜复合材料展示了对 He 和 O2 的选择性分子分离，
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