Qing Qi, Luo Junhan, Liu Shuang, Wang Jingyu, Wang Zhe, Xiong Xiao-Gen, Chen Jing, Lu Yuexiang
Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, China.
Nuclear Research Institute for Future Technology and Policy, Seoul National University, Seoul, Republic of Korea.
Nat Commun. 2025 Mar 15;16(1):2571. doi: 10.1038/s41467-025-57892-6.
Covalent organic frameworks (COFs) are typically synthesized using solvothermal conditions with high temperature and long reaction time (≥120 °C, >72 h). Herein, we report a general and rapid microplasma electrochemistry strategy to synthesize COFs under ambient conditions. A series of flexible imine-bond COFs with high-crystallinity were prepared in minutes via this method, which showed 1000-fold higher space-time yield than solvothermal method. This approach also achieved the preparation of COFs with diverse linkages including rigid imine, hydrazone, β-ketoenamies and azine linkages. Moreover, four types of imine-based COFs were successfully synthesized in aqueous acetic acid, which avoided the use of harmful organic solvents, indicating that microplasma method is green and versatile for COF synthesis. The obtained COFs showed higher surface area and exhibited superior performance in volatile iodine uptake compared to those COFs prepared by solvothermal method. After screening more than ten types of COFs, the iodine adsorption capacity could be promoted from 2.81 to 6.52 g g. The efficiency, versatility, and simplicity of the microplasma method render it as a promising approach for the swift screening of COFs across a wide range of applications.
共价有机框架材料(COFs)通常是在高温和长反应时间(≥120°C,>72小时)的溶剂热条件下合成的。在此,我们报告了一种通用且快速的微等离子体电化学策略,用于在环境条件下合成COFs。通过该方法在数分钟内制备了一系列具有高结晶度的柔性亚胺键COFs,其时空产率比溶剂热法高1000倍。该方法还实现了具有多种连接方式的COFs的制备,包括刚性亚胺、腙、β-酮烯胺和嗪连接。此外,在乙酸水溶液中成功合成了四种类型的亚胺基COFs,避免了使用有害有机溶剂,这表明微等离子体法对于COF合成来说是绿色且通用的。与通过溶剂热法制备的COFs相比,所获得的COFs具有更高的比表面积,并且在挥发性碘吸收方面表现出优异的性能。在筛选了十多种类型的COFs后,碘吸附容量可以从2.81提高到6.52 g/g。微等离子体法的效率、通用性和简便性使其成为一种有前途的方法,可用于快速筛选适用于广泛应用的COFs。