
近日,中山大学潘梅团队研究了热适应闪烁体的高水稳定性铀酰簇基金属有机骨架。2026年3月26日,《美国化学会志》发表了这一成果。
近年来,铀基金属有机框架(MOFs)因铀原子具有可及的5f轨道和多样化的配位几何构型,加之MOFs自身固有的可调性与功能性,而受到特别关注。
研究组报道了一种具有四核铀酰簇结构和独特热适应性闪烁特性的二维MOF材料(UO-TTP)。UO-TTP展现出宽吸收带,并可通过多种途径被激发,涵盖X射线激发及单/双光子激发。在室温下,UO-TTP呈现以550 nm为中心的连续发射峰,该发射源于具有杂化电荷转移特性的激发三重态,其衰减寿命长达约20 ms。然而在低温下,其发射光谱分裂为指状峰,寿命却出人意料地缩短至微秒级。这种热适应性发射开关现象也首次通过X射线激发发光(XEL)得以证实。
此外,UO-TTP表现出优异的稳定性,即使在水浸泡后其发光性能也无显著减弱,在线性响应、检测限和稳定性等方面均表现出作为合格闪烁体的性能。基于UO-TTP卓越的光学特性,研究组创新性地探索了该铀有机框架(UOF)在温度-时间双关联信息加密及热水条件下X射线成像中的应用。这项工作不仅揭示了发光铀有机框架的独特性和优势,也为锕系化学的深入研究铺平了道路。
附:英文原文
Title: Highly Water-Stable Uranyl-Cluster Based Metal–Organic Framework for Thermal Adaptive Scintillator
Author: Rui-Qi Huang, Shao-Zhe Yi, Wen He, Ren-Fu Li, Ya-Nan Fan, Cheng-Yong Su, Mei Pan
Issue&Volume: March 26, 2026
Abstract: In recent years, uranium-based metal–organic frameworks (MOFs) have garnered particular attention due to the accessible 5f orbitals and diverse coordination geometries of the U atom, as well as the tunability and functionality inherent to MOFs. Herein, we report a 2D-MOF (UO-TTP) featuring a tetranuclear uranyl cluster structure and unique thermal adaptive scintillating characters. UO-TTP exhibits a broad absorption band and can be excited through multiple pathways, from X-ray to one/two-photon excitation. At room temperature, UO-TTP exhibits a continuous emission peak centered at 550 nm, originating from the excited triplet states with hybrid CT characteristics and a long decay lifetime of ~20 ms. However, at low temperatures, the emission spectra split into finger-type peaks, with lifetimes unexpectedly shortened to microsecond level. This thermal adaptive emission switch was also detected by X-ray excited luminescence (XEL) for the first time. Moreover, UO-TTP shows outstanding stability, with no significant weakening of its luminescence even after soaked in water, and manifests itself as a qualified scintillator in terms of linear response, detection limit, and stability. Based on the excellent optical properties of UO-TTP, we innovatively explored the application of this uranium-organic framework (UOF) in temperature–time dual-correlated information encryption and X-ray imaging under hot water conditions. This work not only reveals the uniqueness and advantages of luminescent UOFs, but also paves the way for in-depth research into actinide chemistry.
DOI: 10.1021/jacs.5c22949
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c22949
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000
