Shanmugaraju Sankarasekaran, Dabadie Charlyne, Byrne Kevin, Savyasachi Aramballi J, Umadevi Deivasigamani, Schmitt Wolfgang, Kitchen Jonathan A, Gunnlaugsson Thorfinnur
School of Chemistry and Trinity Biomedical Sciences Institute (TBSI) , Trinity College Dublin , The University of Dublin , Dublin 2 , Ireland . Email:
School of Chemistry and Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) , Trinity College Dublin , The University of Dublin , Dublin 2 , Ireland.
Chem Sci. 2017 Feb 1;8(2):1535-1546. doi: 10.1039/c6sc04367d. Epub 2016 Oct 25.
A V-Shaped 4-amino-1,8-napthalimide derived tetracarboxylic acid linker (; bis-[-(1,3-benzenedicarboxylic acid)]-9,18-methano-1,8-naphthalimide-[,][1,5]diazocine) comprising the Tröger's base (TB) structural motif was rationally designed and synthesised to access a nitrogen-rich fluorescent supramolecular coordination polymer. By adopting the straight forward precipitation method, a new luminescent nanoscale Zn(ii) coordination polymer () was synthesized in quantitative yield using Zn(OAc)·2HO and tetraacid linker (1 : 0.5) in DMF at room temperature. The phase-purity of as-synthesised was confirmed by X-ray powder diffraction analysis, infra-red spectroscopy, and elemental analysis. Thermogravimetric analysis suggests that is thermally stable up to 330 °C and the morphological features of was analysed by SEM and AFM techniques. The N adsorption isotherm of thermally activated at 77 K revealed a type-II reversible adsorption isotherm and the calculated Brunauer-Emmett-Teller (BET) surface area was found to be 72 m g. Furthermore, displayed an excellent CO uptake capacity of 76 mg g at 273 K and good adsorption selectivity for CO over N and H. The aqueous suspension of as-synthesized showed strong green fluorescence ( = 520 nm) characteristics due to the internal-charge transfer (ICT) transition and was used as a fluorescent sensor for the discriminative sensing of nitroaromatic explosives. The aqueous suspension of showed the largest quenching responses with high selectivity for phenolic-nitroaromatics (4-NP, 2,4-DNP and PA) even in the concurrent presence of other potentially competing nitroaromatic analytes. The fluorescence titration studies also provide evidence that detects picric acid as low as the parts per billion (26.3 ppb) range. Furthermore, the observed fluorescence quenching responses of towards picric acid were highly reversible. The highly selective fluorescence quenching responses including the reversible detection efficiency make the nanoscale coordination polymer a potential material for the discriminative fluorescent sensing of nitroaromatic explosives.
一种基于V形4-氨基-1,8-萘二甲酰亚胺的四羧酸连接体（即双-[-(1,3-苯二甲酸)]-9,18-亚甲基-1,8-萘二甲酰亚胺-[,][1,5]二氮杂辛），其包含特罗格碱（TB）结构单元，通过合理设计与合成，用于制备一种富氮荧光超分子配位聚合物。采用直接沉淀法，在室温下于N,N-二甲基甲酰胺（DMF）中，以醋酸锌二水合物（Zn(OAc)₂·2H₂O）与四酸连接体（比例为1 : 0.5），以定量产率合成了一种新型发光纳米级锌（II）配位聚合物（）。通过X射线粉末衍射分析、红外光谱和元素分析确认了合成产物的相纯度。热重分析表明，在高达330 °C的温度下热稳定，并用扫描电子显微镜（SEM）和原子力显微镜（AFM）技术分析了其形态特征。在77 K下对热活化后的进行氮气吸附等温线测定，结果显示为II型可逆吸附等温线，计算得到的布鲁诺尔-埃米特-泰勒（BET）表面积为72 m²/g。此外，在273 K下对一氧化碳的吸附容量高达76 mg/g，且对一氧化碳相对于氮气和氢气具有良好的吸附选择性。合成产物的水悬浮液由于内电荷转移（ICT）跃迁而表现出强烈的绿色荧光（发射波长λem = 520 nm）特性，并用作鉴别硝基芳香族炸药的荧光传感器。的水悬浮液对酚类硝基芳烃（4-硝基苯酚、2,4-二硝基苯酚和苦味酸）表现出最大的猝灭响应和高选择性，即使在同时存在其他潜在竞争硝基芳香族分析物的情况下也是如此。荧光滴定研究还证明，能够检测低至十亿分之（26.3 ppb）范围的苦味酸。此外，观察到对苦味酸的荧光猝灭响应具有高度可逆性。包括可逆检测效率在内的高选择性荧光猝灭响应，使得纳米级配位聚合物成为鉴别硝基芳香族炸药的潜在荧光传感材料。
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