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水解稳定的锆基金属有机框架作为放射性核素的高灵敏度和选择性发光传感器

Hydrolytically Stable Zr-Based Metal-Organic Framework as a Highly Sensitive and Selective Luminescent Sensor of Radionuclides.

作者信息

Li Zi-Jian, Wang Xue, Zhu Lin, Ju Yu, Wang Zeru, Zhao Qian, Zhang Zhi-Hui, Duan Tao, Qian Yuan, Wang Jian-Qiang, Lin Jian

机构信息

Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, 2019 Jia Luo Road, Shanghai 201800, P. R. China.

Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Changzhou University, No. 1, Gehu Middle Road, Changzhou 213164, P. R. China.

出版信息

Inorg Chem. 2022 May 16;61(19):7467-7476. doi: 10.1021/acs.inorgchem.2c00545. Epub 2022 May 5.

Abstract

Effective detections of radionuclides including uranium and its predominant fission products, for example, iodine, are highly desired owing to their radiotoxicity and potential threat to human health. However, traditional analytical techniques of radionuclides are instrument-demanding, and chemosensors targeted for sensitization of radionuclides remain limited. In this regard, we report a sensitive and selective sensor of UO and I based on the unique quenching behavior of a luminescent Zr-based metal-organic framework, ZrO(OH)(OH)(HO)(TCPE)·(HO)(CHNO) (). Immobilization of the luminescent tetrakis(4-carboxyphenyl)ethylene (TCPE) linkers by Zr nodes enhances the photoluminescence quantum yield of , which facilitates the effective sensing of radionuclides in a "turn-off" manner. Moreover, can sensitively and selectively recognize UO and I ions with the lowest limits of detection of 0.67 and 0.87 μg/kg, respectively, of which the former one is much lower than the permissible value (30 μg/L) defined by the U.S. EPA. In addition, features excellent hydrolytic stability and can withstand pH conditions ranging from 3 to 11. To facilitate real-world applications, we have further fabricated polyvinylidene fluoride-integrating as luminescence-based sensor membranes for on-site sensing of UO and I.

摘要

由于铀及其主要裂变产物(例如碘)具有放射性毒性以及对人类健康的潜在威胁,因此非常需要对包括铀及其主要裂变产物在内的放射性核素进行有效检测。然而,传统的放射性核素分析技术对仪器要求较高,并且针对放射性核素敏化的化学传感器仍然有限。在这方面,我们基于发光的锆基金属有机框架ZrO(OH)(OH)(HO)(TCPE)·(HO)(CHNO)()的独特猝灭行为,报道了一种对UO和I敏感且具有选择性的传感器。Zr节点对发光的四(4-羧基苯基)乙烯(TCPE)连接体的固定提高了其光致发光量子产率,这有助于以“关闭”方式有效检测放射性核素。此外,该传感器能够分别以最低检测限0.67和0.87μg/kg灵敏且选择性地识别UO和I离子,其中前者远低于美国环境保护局规定的允许值(30μg/L)。此外,该传感器具有出色的水解稳定性,能够承受pH值范围为3至11的条件。为了便于实际应用,我们进一步制备了集成该传感器的聚偏二氟乙烯发光传感器膜,用于现场检测UO和I。

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