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Unveiling the Uncommon Fluorescent Recognition Mechanism towards Pertechnetate Using a Cationic Metal–Organic Framework Bearing N‐Heterocyclic AIE Molecules
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2021-01-27 , DOI: 10.1002/chem.202005362
Kang Kang 1 , Xing Dai 2 , Nannan Shen 2 , Rongzhen Xie 2 , Xingwang Zhang 1 , Lecheng Lei 1 , Shuao Wang 2 , Chengliang Xiao 3
Affiliation  

As one of most problematic radionuclides, technetium‐99, mainly in the form of anionic pertechnetate (TcO4), exhibits high environmental mobility, long half‐life, and radioactive hazard. Due to low charge density and high hydrophobicity for this tetrahedral anion, it is extremely difficult to recognize it in water. Seeking efficient and selective recognition method for TcO4 is still a big challenge. Herein, a new water‐stable cationic metal‐organic framework (ZJU‐X8) was reported, bearing tetraphenylethylene pyrimidine‐based aggregation‐induced emission (AIE) ligands and attainable silver sites for TcO4 detection. ZJU‐X8 underwent an obvious spectroscopic change from brilliant blue to flavovirens and exhibited splendid selectivity towards TcO4. This uncommon fluorescent recognition mechanism was well elucidated by batch sorption experiments and DFT calculations. It was found that only TcO4 could enter into the body of ZJU‐X8 through anion exchange whereas other competing anions were excluded outside. Subsequently, after interaction between TcO4 and silver ions, the electron polarizations from pyrimidine rings to Ag+ cations significantly lowered the energy level of the π* orbital and thus reduced the π–π* energy gap, resulting in a red‐shift in the fluorescent spectra.

中文翻译:

利用带有N杂环AIE分子的阳离子金属有机骨架揭示高Per酸酯的罕见荧光识别机制

作为最成问题的放射性核素的一个,锝-99,主要是在阴离子高锝酸盐的形式(TCO 4 - ),显示出高流动性的环境,半衰期长,以及放射性危害。由于该四面体阴离子的电荷密度低且疏水性高,因此在水中很难识别。寻求TCO效率和选择性识别方法4 -仍然是一个很大的挑战。本文报道了一种新的水稳定性阳离子金属有机骨架(ZJU-X8),带有四苯基乙烯嘧啶基聚集诱导发射(AIE)配体和可达到的TcO 4的银位点-检测。ZJU-X8经历了从辉煌的蓝色明显光谱变化flavovirens和对TCO表现出色的选择性,4 - 。通过批吸附实验和DFT计算可以很好地阐明这种不常见的荧光识别机制。结果发现,只有TCO 4 -可以通过阴离子交换进入ZJU-X8的身体,而其他竞争性阴离子被排除之外。随后,TCO之间相互作用后4 -离子和银离子,从嘧啶环,以银的电子偏振+阳离子显著降低了π的能级*轨道,从而降低了π-π*能隙,从而在红移荧光光谱。
更新日期:2021-03-27
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