School for Radiological and interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, 199 Ren'ai Road, Suzhou, 215123, China.
High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei, Anhui, 230031, China.
Angew Chem Int Ed Engl. 2017 Jun 19;56(26):7500-7504. doi: 10.1002/anie.201700919. Epub 2017 May 19.
Precise detection of low-dose X- and γ-radiations remains a challenge and is particularly important for studying biological effects under low-dose ionizing radiation, safety control in medical radiation treatment, survey of environmental radiation background, and monitoring cosmic radiations. We report here a photoluminescent uranium organic framework, whose photoluminescence intensity can be accurately correlated with the exposure dose of X- or γ-radiations. This allows for precise and instant detection of ionizing radiations down to the level of 10 Gy, representing a significant improvement on the detection limit of approximately two orders of magnitude, compared to other chemical dosimeters reported up to now. The electron paramagnetic resonance analysis suggests that with the exposure to radiations, the carbonyl double bonds break affording oxo-radicals that can be stabilized within the conjugated uranium oxalate-carboxylate sheet. This gives rise to a substantially enhanced equatorial bonding of the uranyl(VI) ions as elucidated by the single-crystal structure of the γ-ray irradiated material, and subsequently leads to a very effective photoluminescence quenching through phonon-assisted relaxation. The quenched sample can be easily recovered by heating, enabling recycled detection for multiple runs.
精确探测低剂量 X 射线和 γ 射线仍然是一个挑战,这对于研究低剂量电离辐射下的生物效应、医学辐射治疗中的安全控制、环境辐射背景调查以及监测宇宙辐射等方面尤为重要。我们在此报告了一种发磷光的铀有机框架,其发光强度可以与 X 射线或 γ 射线的辐射剂量精确相关。这使得精确、即时的电离辐射探测成为可能,其探测下限可低至 10 Gy,与迄今为止报道的其他化学剂量计相比,探测限提高了约两个数量级。电子顺磁共振分析表明,随着辐射的暴露,羰基双键断裂,生成可以在共轭铀草酸盐-羧酸盐片中稳定存在的氧自由基。这导致了铀酰(VI)离子的赤道键合大大增强,这可以通过γ射线辐照材料的单晶结构阐明,随后通过声子辅助弛豫导致非常有效的磷光猝灭。通过加热可以很容易地使猝灭的样品恢复,从而实现多次运行的可回收检测。