2026年“核理安邦”联合博士生学术论坛

MIPEC诱导高碘吸附性能共价有机框架的超快合成

Not scheduled

1h

地址：清华大学校内

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Speaker

琪 卿

摘要

共价有机框架（COFs）作为一类晶态多孔有机材料，因具有高比表面积、可调控孔道结构、丰富的活性位点及优异的化学稳定性，在放射性碘吸附领域展现出巨大应用潜力。然而，传统 COFs 合成方法（如溶剂热法）条件较为严苛（≥ 120℃，72 h），严重制约了其规模化制备与实际应用。开发一种高效、绿色、通用的COFs快速合成方法，作为筛选高性能碘吸附COFs材料的筛选平台，对保障环境安全与核能可持续发展具有重要意义。基于微等离子体电化学方法（MIPEC）的COFs快速合成策略，实现了室温常压下COFs的高效制备，所合成材料具有良好结晶性以及高比表面积。进一步对MIPEC合成 COFs机理进行了深入探索，结果表明微等离子体产生的高能活性物种对于引发和加速合成反应具有重要作用，同时水可以促进结晶。相比于传统的溶剂热方法，MIPEC方法具有低能耗与高时空产率，能耗较溶剂热法降低五个数量级，时空产率高千倍，为现有报道时空产率最高的方法之一。此外，MIPEC具有一定的通用性，成功合成多种柔性亚胺键COFs及不同键型（刚性亚胺键、腙键、烯酮-胺键、吖嗪键）的COFs，且适用于乙酸水溶液中亚胺基COFs的制备，避免有毒有机溶剂的使用。所合成材料性能优异，且热稳定性良好，为碘吸附应用提供了候选材料。基于MIPEC的超快合成平台，既可以合成碘吸附性能优异的COFs材料，同时提供了一种快速的高通量筛选方式，为未来新型COFs材料的设计与理论计算筛选提供参考数据。

Abstract

Covalent organic frameworks (COFs), as an emerging class of crystalline porous organic materials, have shown remarkable potential for radioactive iodine capture due to their high specific surface area, tunable pore structures, abundant active sites, and excellent chemical stability. However, conventional synthesis methods, such as solvothermal approaches, typically require harsh conditions (≥ 120℃) and long reaction times (72 h), which significantly hinder their scalable production and practical application. Therefore, it’s necessary to develop an efficient, green, and generalizable method for rapid COFs synthesis. In this study, we propose a rapid synthesis and screening strategy for COFs based on microplasma electrochemistry (MIPEC), enabling efficient preparation of COFs under ambient temperature and pressure, along with systematic evaluation of their iodine adsorption performance. The synthesis mechanism of MIPEC was explored further, the highly reactive species generated by the microplasma effectively initiate and accelerate the synthesis reactions. Compared to conventional solvothermal methods, the MIPEC approach exhibits notable energy-saving advantages and exceptionally high space-time yield. This method demonstrates good generality, having been successfully applied to synthesize a series of COFs with flexible imine linkages and COFs with diverse linkages (rigid imine, hydrazone, β-ketoenamies and azine linkages). The ultrafast synthesis platform based on MIPEC can be used for high-throughput screening of high-performance COFs for iodine capture. The MIPEC method not only enables the synthesis of materials with superior iodine adsorption performance but also offers an efficient screening pathway, providing valuable reference data for the rational design and computational screening of novel COFs in the future.