基于合成后修饰策略构建高灵敏度和选择性金属有机骨架基荧光静默系统用于抗坏血酸的检测 |
Assembling a luminescence silencing system based on post-synthetic modification strategy: A highly sensitive and selective turn-on metal-organic framework probe for ascorbic acid detection |
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摘要: 成功制备了一种在水溶液中表现出优异荧光性能和稳定结构的三维荧光金属有机骨架[Cd (L)(H2O)0.5]·DMF·2.5H2O (1),其中H2L=3-(四唑-5-基)三唑。1在识别Cr (Ⅵ)离子过程中表现出明显的荧光猝灭现象,并形成“开-关”荧光静默体系(Cr2O72-@1),该体系可以快速检测水溶液中的Cr (Ⅵ)离子,这是Cr (Ⅵ)的紫外吸收光谱和1的激发光谱重叠而导致的福斯特共振能量转移(FRET)。此外,通过消除FRET的作用,Cr2O72-@1的荧光强度可以恢复或超越原始值,从而实现对水体系中抗坏血酸(AA)的高选择性和灵敏度的荧光检测。同时,Cr2O72-@1体系可以成功检测维生素C片中的AA,回收率为98.20%~103.33%,相对标准偏差(RSD)为1.78%~3.42%。基于此,构建了以AA和铬(Ⅵ)为化学输入的荧光“IMPLICATION”分子逻辑门。 |
关键词: 荧光静默系统 金属有机骨架 Cr(Ⅵ) 抗坏血酸 |
基金项目: 山西省自然科学基金(No. 202203021212331)、山西省高校科技创新项目(No. 2022L532)、安徽高校自然科学研究重大项目(No. 2022AH040142)和安徽省高校优秀青年项目(No. 2022-194)资助。 |
Abstract: A unique 3D luminescent metal - organic framework, namely [Cd(L) (H2O)0.5]·DMF·2.5H2O (1), where H2L=3-(tetrazol-5-yl)triazole, has been successfully prepared and characterized. The framework has demonstrated excellent luminescence properties and structural stability in the water system. Notably, the luminescence intensity of 1 was significantly quenched by Cr(Ⅵ)(1 mL of Cr2O72- or 150 μL of CrO42-, 1 mmol·L-1), leading to the formation of an“on-off”luminescence silencing system (Cr2O72-@1), which was capable of accurately detecting Cr(Ⅵ) in the water system. The primary mechanism responsible for luminescence quenching was the Forster resonance energy transfer (FRET) process. Additionally, by removing the involvement of the FRET process, the luminescence intensity of the Cr2O72-@1 system could be restored, allowing for the highly selective and sensitive detection of ascorbic acid (AA) in water systems. Moreover, it has been demonstrated that 1 can successfully detect AA in vitamin C tablets, yielding recovery rates ranging from 98.20% to 103.33% and relative standard deviations (RSDs) ranging from 1.78% to 3.42%. Based on the findings of this experiment, a luminescent “IMPLICATION” molecular logic gate has been constructed utilizing AA and Cr(Ⅵ) as the chemical inputs, respectively. |
Keywords: luminescence silencing metal-organic framework Cr(Ⅵ) ascorbic acid |
投稿时间:2023-08-15 修订日期:2024-01-04 |
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张婕,刘欣,李梓欣,裴玉婷,杨宇琦,李慧敏,刘志强.基于合成后修饰策略构建高灵敏度和选择性金属有机骨架基荧光静默系统用于抗坏血酸的检测[J].无机化学学报,2024,40(4):823-833. |
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