阐明ZIF-L中客体-主体机制以实现可调谐高发光二维材料
Elucidating Guest-Host Mechanisms in ZIF-L for Tuneable Highly Luminescent 2D Materials
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中文总结 AI 辅助
本研究通过分析荧光素@ZIF-L和苝@ZIF-L，阐明了二维ZIF-L中客体掺入机制，实现了可调谐高发光性能（量子产率99.7%）及白光发射，并展示了原位薄膜制备技术。
中文摘要 AI 辅助
三维金属有机框架（MOFs）是众所周知的发光客体的有效主体，能够提高可调谐性、光稳定性和材料可加工性。二维客体@MOF体系虽然研究较少，但由于其光学透明性、层间间距和垂直薄度，相比三维客体@MOF体系具有竞争优势。本研究考察了发光有机染料@ZIF-L，以建立ZIF-L中客体掺入的基本机制，并展示二维ZIF-L结构在材料功能性发光方面的优势。通过分析案例研究体系荧光素@ZIF-L（F@ZIF-L），使用纳米级傅里叶变换红外光谱、衍射和拓扑映射，确认了荧光素（F）位于ZIF-L框架空腔中。在表面能模拟的支持下，发现客体掺入程度由形态连续体指示，从特征性的叶状ZIF-L到矩形F@ZIF-L。通过改变合成温度和溶剂比例，F@ZIF-L的发光性质可以在客体负载量（摩尔百分比）和排列（即客体单体与聚集体比例）方面进行理性调控。优化后，F@ZIF-L表现出可调谐的发射色度、99.7%的光致发光量子产率、在溶液中12个月内极小的客体浸出以及高光稳定性。苝@ZIF-L表现出独特的白光发射特性，其CIE坐标（0.33, 0.34）源于黄色α相激基复合物和蓝色单体苝发射的组合。最后，在可延展的锌箔上生长了取向性发光客体@ZIF-L材料薄膜，展示了一种原位制备技术。总之，这项工作突出了发光染料@ZIF-L体系在开发下一代光电子学、传感器和照明系统中可调谐且耐用的发光组件方面的潜力。
英文摘要
3D metal-organic frameworks (MOFs) are well known effective hosts for luminescent guests that improve tuneability, photostability and material fabricability. 2D guest@MOF systems, while less explored, offer competitive advantages over 3D guest@MOF systems due to their optical transparency, inter-layer spacing, and vertical thinness. This work examines luminescent organic dyes@ZIF-L to establish the underlying mechanisms of guest incorporation in ZIF-L and demonstrate the advantages of the 2D ZIF-L architecture for the material's functional luminescence. Analysing a case study system, fluorescein@ZIF-L (F@ZIF-L), using nanoscale FTIR, diffraction, and topology mapping, confirmed that fluorescein (F) resided in the ZIF-L framework cavities. Supported by surface energy simulations, the extent of guest incorporation was found to be indicated by a morphological continuum, from the characteristic leaf-shaped ZIF-L to rectangular F@ZIF-L. By modifying synthesis temperature and solvent ratios, the luminescent properties of F@ZIF-L could be rationally tuned in terms of guest loading (% mol) and arrangement (i.e. guest monomer to aggregate ratio). When optimised, F@ZIF-L exhibited tuneable emission chromaticity, 99.7% photoluminescent quantum yield, minimal guest leaching in solution over 12 months, and high photostability. Perylene@ZIF-L exhibited unique white light emitting properties, with CIE coordinates (0.33, 0.34) arising from a combination of yellow alpha-phase excimer and blue monomeric perylene emission. Finally, oriented luminescent thin films of guest@ZIF-L materials were grown on malleable Zn foils, demonstrating an in situ fabrication technique. Together, the work highlights the potential for luminescent dye@ZIF-L systems in developing tuneable and resilient luminescent components of next-generation optoelectronics, sensors, and lighting systems.
发表机构
- University of Oxford（牛津大学）
- University of Turin（都灵大学）
- Attocube Systems AG（阿托库伯系统股份公司）
- Universidad de Alicante（阿利坎特大学）
- Diamond Light Source Ltd.（钻石光源有限公司）
机构由 AI 辅助整理，请以论文原文为准。
