Fluorinated Eu(II)-based multimodal contrast agent for temperature- and redox-responsive magnetic resonance imaging.

Fluorinated Eu(II)-based multimodal contrast agent for temperature- and redox-responsive magnetic resonance imaging.
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DOI:
10.1039/c7sc03142d
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发表时间:
2017-12-01
期刊:
影响因子:
8.4
通讯作者:
Allen MJ
Allen MJ
中科院分区:
化学1区
文献类型:
--
作者:
Basal LA;Bailey MD;Romero J;Ali MM;Kurenbekova L;Yustein J;Pautler RG;Allen MJ

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机制上独特的19F-EuII/III复合物使用1H-和19F-MRI报告体内氧化还原,并显示温度依赖的对比度增强。磁共振成像(MRI)使用氧化还原活性,含euii复合物是最有前途的无创成像缺氧在体内的技术之一。在该技术中,在氧化能力相对较低的区域,如缺氧组织,阳性(t1加权)对比增强持续存在。在这里,我们描述了一种含氟的euii配合物,其中氧化还原活性金属通过分子内相互作用被笼化。氟原子的位置使造影剂还原形式的温度响应造影剂增强和通过MRI在体内检测氧化造影剂成为可能。Eu为+2氧化态时,1H-MRI表现为正对比;Eu为+3氧化态时,19F-MRI表现为化学交换饱和转移和信号。对比度增强由Eu的氧化还原状态控制,并由束缚水分子以温度依赖的方式降低弛豫度的氟相互作用调节。总之,这些进展构成了使用19F-MRI进行体内氧化还原反应成像的第一份报告。
Mechanistically unique 19F-EuII/III complex reports redox in vivo using both 1H- and 19F-MRI and displays temperature-dependent contrast enhancement. Magnetic resonance imaging (MRI) using redox-active, EuII-containing complexes is one of the most promising techniques for noninvasively imaging hypoxia in vivo. In this technique, positive (T1-weighted) contrast enhancement persists in areas of relatively low oxidizing ability, such as hypoxic tissue. Herein, we describe a fluorinated, EuII-containing complex in which the redox-active metal is caged by intramolecular interactions. The position of the fluorine atoms enables temperature-responsive contrast enhancement in the reduced form of the contrast agent and detection of the oxidized contrast agent via MRI in vivo. Positive contrast is observed in 1H-MRI with Eu in the +2 oxidation state, and chemical exchange saturation transfer and 19F-MRI signal are observed with Eu in the +3 oxidation state. Contrast enhancement is controlled by the redox state of Eu, and modulated by the fluorous interactions that cage a bound water molecule reduce relaxivity in a temperature-dependent fashion. Together, these advancements constitute the first report of in vivo, redox-responsive imaging using 19F-MRI.
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