从客体诱导结晶到分子印记:以计算为导向的发现,为p-xylen分离提供了与结合的四醇框架
Yi Su1, Qiang Gao2, Xiaojun Ding1
1Collaborative Innovation Center of Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology, Tsinghua University, 100084, Beijing, China.
一个新的客人诱导的结晶策略成功地创造了具有挑战性的多孔结有机框架 (HOF). 这种方法使得可预测的组装有孔的晶体材料进行选择性分离.
科学领域:
- 材料科学 材料科学 材料科学
- 超分子化学 超分子化学
- 晶体学 晶体学是指结晶学.
背景情况:
- 主机-客户互动是设计多孔晶体材料 (PCM) 的关键.
- 一个主要的挑战是识别客人,以防止密集包装,并使多孔性.
- 结构复杂的建筑单元阻碍了新型多孔框架的发展.
研究的目的:
- 开发一种客体诱导结晶 (GIC) 策略,用于创建多孔的键有机框架 (HOF).
- 使用热力学计算来指导HOF合成的客人选择.
- 探索GIC衍生HOF在C8芳香异构体分离中的应用.
主要方法:
- 热力学计算,包括形成能量 (ΔE) 的密度函数理论 (DFT).
- 晶体结构分析以确定GIC的热力学原理.
- 使用四醇构件的新型HOFs的合成和表征.
- 气体和液体吸附实验,以评估分离性能.
主要成果:
- 一个新的GIC策略成功合成了动力学上具有挑战性的HOFs.
- 在GIC.中为客人选择建立了热力学标准.
- 在客人诱导的HOF中,比其他C8芳香物对p-xylen (PX) 具有很高的选择性.
- 一个没有客人的HOF,HOF-PX-a,在液体吸附中表现出PX/乙 (21.7) 的记录选择性.
结论:
- 该研究阐明了HOF结构中GIC的自组装规则.
- 这种方法使PCM可预测的组装用于分子识别.
- GIC为设计针对特定目标的分离的先进多孔材料提供了新的机会.
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