镧-钛氧簇闪烁体中无机簇核和有机配体的协同作用实现高性能X射线成像  

The synergy of inorganic cluster cage and organic ligands in lanthanide-titanium-oxo clusters scintillators for high performance X-ray imaging

作　　者：李茹画 桑天天 曹钱 刘娟 倪京飞 王超 刘淑娟 刘湘梅 赵强 Ruhua Li;Tiantian Sang;Qian Cao;Juan Liu;Jingfei Ni;Chao Wang;Shujuan Liu;Xiangmei Liu;Qiang Zhao(State Key Laboratory of Organic Electronics and Information Displays&Jiangsu Key Laboratory of Smart Biomaterials and Theranostic Technology,Institute of Advanced Materials,Nanjing University of Posts and Telecommunications,Nanjing 210023,China;College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology),Nanjing University of Posts&Telecommunications,Nanjing 210023,China;Shanxi Open University,Taiyuan 030027,China)

机构地区：[1]State Key Laboratory of Organic Electronics and Information Displays&Jiangsu Key Laboratory of Smart Biomaterials and Theranostic Technology,Institute of Advanced Materials,Nanjing University of Posts and Telecommunications,Nanjing 210023,China [2]College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology),Nanjing University of Posts&Telecommunications,Nanjing 210023,China [3]Shanxi Open University,Taiyuan 030027,China

出　　处：《Science China Materials》2024年第8期2575-2582,共8页中国科学（材料科学）（英文版）

基　　金：the financial support from the National Key R&D Program of China(2023YFE0202500);the National Funds for Distinguished Young Scientists(61825503);the National Natural Science Foundation of China(22161160318 and 62275129);the Project of State Key Laboratory of Organic Electronics and Information Displays,Nanjing University of Posts&Telecommunications(GZR2023010008)。

摘　　要：随着对X射线成像,特别是对弯曲和不规则物体的三维成像的需求不断增加,高性能柔性闪烁膜的开发引起了人们的极大关注.镧系(Ⅲ)-有机闪烁体由于其在结构设计和光学可调谐方面的巨大灵活性,最近成为一类新的有前途的X射线闪烁体.然而,设计具有高光产额和良好溶液分散性的镧系元素(Ⅲ)-有机闪烁体仍然具有挑战性.本文报道了一种具有高效X射线激发发光(XEL)和良好溶液分散性的铕-钛氧簇合物(Eu-TiOCs)闪烁体.笼状镧-钛氧原子簇核作为X射线吸收剂,产生高能电子并引发二次电子热弛豫.有机配体作为能量转移桥和天线,通过级联能量转移来敏化Ln^(3+);离子的发光.Eu-TiOCs闪烁体表现出高的稳态X射线光产额(高达26,816±2000 photons MeV^(-1)).此外,EuTiOCs闪烁体和聚合物的羟基之间的弱氢键相互作用增强了Eu-TiOCs的溶液分散性,有利于制备低光散射和均匀闪烁膜.铕-钛氧簇与聚合物之间的通过无机簇笼和有机配体之间的协同作用,所得到的柔性闪烁膜对平面和非平面物体都表现出的高空间分辨率和低剂量X射线成像.本工作为进一步设计和制备高性能X射线闪烁体和高分辨率柔性闪烁膜提供了新思路.With the increasing demand for X-ray imaging,especially for three-dimensional imaging of curved and irregular objects,the development of high-performance flexible scintillation films has attracted significant interest.Lanthanide(III)-organic scintillators have recently emerged as a new promising class of X-ray scintillators for their great flexibility in structural design and optical tuning.However,designing lanthanide(III)-organic scintillators with high light yields and good solution dispersibility is still challenging.Herein,a europium-titanium oxo cluster(Eu-TiOC)scintillator with highly-efficient X-ray excited luminescence and good solution dispersibility is reported.The cage-like lanthanide-titanium oxo cores served as X-ray absorbers to produce high-energy electrons,initiating secondary electron thermal relaxation.Organic ligands functioned as energy transfer bridges and antennas,sensitizing Ln3+ions’luminescence through cascaded energy transfer processes.As a result,the Eu-TiOCs scintillator exhibited high steady-state X-ray light yields(up to 26,816±2000 photons MeV−1).In addition,the weak hydrogen bonding interaction between the Eu-TiOCs and the polymer enhanced the solution dispersibility of Eu-TiOCs,facilitating the preparation of low light-scattering and uniform scintillation films.By the synergy between the inorganic cluster cage and organic ligands,the resulting flexible scintillation film achieved a high spatial resolution of 12.8 lp mm−1 and enabled low-dose X-ray imaging for both planar and non-planar objects.

关 键 词：X射线成像 不规则物体 有机配体 能量转移 二次电子 闪烁体 高能电子 热弛豫 

分 类 号：O434.19[机械工程—光学工程] TP391.41[理学—光学] O641.4[理学—物理]