Liu Hanzhou, Qin Haoming, Shen Nannan, Yan Siqi, Wang Yaxing, Yin Xuemiao, Chen Xinjian, Zhang Chao, Dai Xing, Zhou Ruhong, Ouyang Xiaoping, Chai Zhifang, Wang Shuao
State Key Laboratory of Radiation Medicine and Protection, School for Radiological and interdisciplinary Sciences (RAD-X), and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou, 215123, China.
Advanced Research Institute for Multidisciplinary Science, Qilu University of Technology (Shandong Academy of Sciences), Jinan, 250353, China.
Angew Chem Int Ed Engl. 2020 Aug 24;59(35):15209-15214. doi: 10.1002/anie.202006380. Epub 2020 Jun 17.
Radio-photoluminescence (RPL) materials display a distinct radiation-induced permanent luminescence center, and therefore find application in the detection of ionizing radiation. The current inventory of RPL materials, which were discovered by serendipity, has been limited to a small number of metal-ion-doped inorganic materials. Here we document the RPL of a metal-organic framework (MOF) for the first time: X-ray induced free radicals are accumulated on the organic linker and are subsequently stabilized in the conjugated fragment in the structure, while the metal center acts as the X-ray attenuator. These radicals afford new emission features in both UV-excited and X-ray excited luminescence spectra, making it possible to establish linear relationships between the radiation dose and the normalized intensity of the new emission feature. The MOF-based RPL materials exhibit advantages in terms of the dose detection range, reusability, emission stability, and energy threshold. Based on a comprehensive electronic structure and energy diagram study, the rational design and a substantial expansion of candidate RPL materials can be anticipated.
放射性光致发光（RPL）材料具有独特的辐射诱导永久性发光中心，因此在电离辐射检测中得到应用。目前通过偶然发现的RPL材料库存仅限于少数金属离子掺杂的无机材料。在此，我们首次记录了金属有机框架（MOF）的RPL：X射线诱导的自由基在有机连接体上积累，随后在结构中的共轭片段中稳定下来，而金属中心充当X射线衰减器。这些自由基在紫外激发和X射线激发的发光光谱中都提供了新的发射特征，使得在辐射剂量与新发射特征的归一化强度之间建立线性关系成为可能。基于MOF的RPL材料在剂量检测范围、可重复使用性、发射稳定性和能量阈值方面表现出优势。基于全面的电子结构和能量图研究，可以预期对候选RPL材料进行合理设计并大幅扩展。
