Synergistic regulation of photoluminescence in covalent organic frameworks by linkages and functional groups

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2025-05-15 Epub Date: 2025-03-05 DOI:10.1016/j.micromeso.2025.113579

Lei Fang , Shaoping Feng , Heping Yan , Na Wu , Gaozhang Gou

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Abstract

Covalent organic frameworks (COFs) provide considerable design flexibility concerning linkages and functional groups. By modulating the degree of conjugation, charge delocalization, and π-π stacking of COFs, promising photoluminescent materials can be developed. Here, we synthesized a series of 2D COFs containing aggregation-caused quenching (ACQ) groups (pyrene), and the fluorescence of the pyrene moiety was fine-tuned by varying the linkers (imine, olefin) and functional groups (‒OH, ‒OMe, ‒F). Compared to imine-based COFs, the olefin-linked COF (Olefin-COF-F) exhibited significantly enhanced photoluminescence, with ten times higher quantum efficiency than Imine-COF. Olefin-COF-F benefits from interlayer hydrogen bonding and can detect HCl via fluorescence turn-off behavior and showed fluorescence turn-on behavior in NaOH solutions. Coating blue light-emitting diodes with Olefin-COF-F resulted in a high-purity white-light device. This research offers valuable insights into the controlled synthesis of COF-based photoluminescent materials featuring ACQ groups.

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共价有机框架中键和官能团的光致发光协同调节

共价有机框架（COFs）在连接和官能团方面提供了相当大的设计灵活性。通过调制COFs的共轭度、电荷离域和π-π堆积，可以开发出有前途的光致发光材料。在这里，我们合成了一系列含有聚集引起的猝灭（ACQ）基团（芘）的二维COFs，并通过改变连接基团（亚胺，烯烃）和官能团（-OH, -OMe, -F）来微调芘部分的荧光。与亚胺基COF相比，烯烃链COF（烯烃-COF- f）的光致发光性能显著增强，量子效率比亚胺基COF高10倍。烯烃- cof - f受益于层间氢键，可以通过荧光关闭行为检测HCl，并在NaOH溶液中显示荧光打开行为。在蓝色发光二极管上涂覆烯烃- cof - f，得到了高纯度的白光器件。本研究为ACQ基cof基光致发光材料的受控合成提供了有价值的见解。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.