用于多环芳烃GC分析的纳米孔洞金属-有机骨架膜原位可控制备原理及作用机制研究

Rapid separation and detection of trace Polycyclic Aromatic Hydrocarbons (PAHs) in environment have been challenges in Analytic Chemistry. In this project, nanoporous metal-organic frameworks (MOFs) will be studied comprehensively as a new kind of separation materials. Through investigation of the interaction mechanism between PAHs and MOFs, the structure of the MOFs for selective separation of specific PAHs will be designed. The as-designed MOFs will be stabilized on the inner surface of capillary column to form a thin film via a layer-by-layer self-assembly method, which be employed as a chromatographic stationary phases to study their comprehensive performance, including the column efficiency, the thermal stability, column life，separation efficiency and sorption activity. The effects of the thickness of the film, the structure of the MOFs, and the distribution of active sites on the separation of PAHs will be also investigated. On the basis of the above results, the capillary column and separation operation parameters will be optimized to realize the rapid separation and detection of trace PAHs. Through implementation of the project, several key scientific questions will be clarified, such as the effect of the structure of MOFs, the effect of active sites, the effect and interaction mechanism of hydrogen bond and π-π conjugation between MOFs and PAHs, which will provide development of new MOFs materials chromatographic stationary phases with experimental evidence and theoretical guidance.

环境中痕量多环芳烃（PAHs）的快速分离检测一直是分析化学的难点。本项目拟以纳米孔洞金属-有机骨架（MOFs）新型分离材料作为研究对象，研究PAHs与MOFs分离材料相互作用机制，设计选择性分离PAHs的MOFs材料；通过层层自组装法在毛细管内壁原位制备MOFs材料薄膜并以其作为气相色谱（GC）固定相，测试评价其柱效、热稳定性、柱寿命、分离效率及吸附活性等综合性能；研究MOFs材料薄膜为固定相的GC毛细管柱对PAHs的分离效能，揭示MOFs的膜厚、孔道结构、活性位点等因素对PAHs分离度的影响，优化色谱柱和GC条件，实现PAHs的快速分离。在此研究基础上，阐明MOFs分离材料的孔道结构、活性位点以及PAHs与MOFs之间氢键、π-π共轭等相互作用对PAHs分离效能的影响等关键科学问题，为开发新型MOFs毛细管柱固定相提供实验依据和理论指导。

环境中痕量多环芳烃（PAHs）的快速分离检测一直是分析化学的难点。本项目通过研究PAHs与MOFs材料相互作用机制，设计了选择性分离PAHs的MOFs材料；并通过层层自组装法和流动涂覆法在毛细管内壁制备MOFs材料薄膜；以负载了MOFs材料的毛细管作为气相色谱（GC）固定相，测试评价了柱效、热稳定性、柱寿命、分离效率及吸附活性等综合性能，研究了MOFs材料薄膜为固定相的GC毛细管柱对PAHs的分离效能，结果显示：层层自组装方法制备MOFs薄膜的毛细管在柱效、热稳定性方面表现较好，而涂覆法制备MOFs薄膜的毛细管在吸附活性方面表现较好；在此研究基础上，还进一步探索了MOFs分离材料的孔道结构、活性位点以及PAHs与MOFs之间氢键、π-π共轭等相互作用对PAHs分离效能的影响等关键科学问题，研究结果为开发新型MOFs毛细管柱固定相提供实验依据和理论指导。