用于超长可见化学发光的精密微反应器

IF 7.2 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2024-06-13 DOI:10.1021/acs.chemmater.4c01126
Yutong Wang, Mingyue Fu, Meng Sun, Fugang Li, Fei Gao, Xiaokang Wang, Xinlei Yang, Hongyan Liu, Zhenyu Xiao*, Weidong Fan* and Daofeng Sun, 
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引用次数: 0

摘要

化学发光微反应器(CLMR)将催化中心、发光中心和开放通道整合到一个原子尺度的平台上,与通常的均相溶剂体系相比,它能显著增强光发射。在此,我们报告了一种新型金属有机框架(MOF)--UPC-88,它是由寡氨酰官能化的 H4LIM-2H 配体(4,4′,4″、4‴-((萘-1,4-二基双(4,1-亚苯基))双(1H-咪唑-2,4,5-三基))四苯甲酸)与第一个用于 CLMR 的双(金属/有机)H2O2 催化中心构建而成。由于固定的发色团和集成的双催化位点,弛豫现象大大减少,能量传递效率显著提高,从而使 UPC-88 具有出色的发光性能。据记录,UPC-88 系统的可见光发光时间长达 1100 分钟,是迄今所报道的 MOF 系统中最高的发光时间之一。我们首次对荧光强度和荧光功率进行了线性拟合,结果表明 UPC-88 是目前报道的荧光功率最高的 MOF 化学发光材料。对 CL 反应机理的探索揭示了洛芬碱基中心在过氧化氢分解过程中的关键作用,从而实现了化学能到光能的高效转化。该平台将为下一代 CLMR 系统和改进 CL 性能提供理论和实验基础。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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A Precise Microreactor for Ultralong Visible Chemiluminescence

Chemiluminescence microreactors (CLMR) integrate catalytic centers, luminescent centers, and open channels into an atomic-scale platform, which can provide significantly enhanced light emission compared with usual homogeneous solvent systems. Herein, we report a novel metal–organic framework (MOF), UPC-88, which is constructed by a lophinyl-functionalized H4LIM-2H ligand (4,4′,4″,4‴-((naphthalene-1,4-diylbis(4,1-phenylene))bis(1H-imidazole-2,4,5-triyl))tetrabenzoic acid) with the first double (metal/organic) H2O2 catalytic center for CLMR. Due to the fixed chromophore and integrated dual catalytic sites, the relaxation phenomenon is greatly reduced and the energy transfer efficiency is significantly improved, resulting in the outstanding light emission performance of UPC-88. The visible luminous time of the UPC-88 system up to 1100 min was recorded as one of the highest ever reported for MOF systems. We linearly fitted the fluorescence intensity and fluorescence power for the first time, and the results show that UPC-88 is the MOF chemiluminescent material with the highest fluorescence power reported so far. The exploration of the CL reaction mechanism reveals the key role of the lophine base center in the decomposition of hydrogen peroxide, enabling the efficient conversion of chemical energy to light energy. This platform will provide a theoretical and experimental basis for next-generation CLMR systems and improved CL performance.

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来源期刊
Chemistry of Materials
Chemistry of Materials 工程技术-材料科学:综合
CiteScore
14.10
自引率
5.80%
发文量
929
审稿时长
1.5 months
期刊介绍: The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.
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