Fluorous Liquids for Magnetic Resonance-Based Thermometry with Enhanced Responsiveness and Environmental Degradation
Fluorous Liquids for Magnetic Resonance-Based Thermometry with Enhanced Responsiveness and Environmental Degradation
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DOI：
10.1021/acs.analchem.3c00172
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发表时间：
2023-03-31
影响因子：
7.4
通讯作者：
Pomerantz，William C. K.
中科院分区：
文献类型：
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作者：
Li，Jiaqian;Mundhenke，Thomas F.;Pomerantz，William C. K.
通过磁共振进行准确的温度测量对于局部组织的体外和体内分析都很有价值，可用于评估疾病病理和医疗干预。基于1H MRI的测温法在临床上使用，但容易受到磁场漂移和脂肪组织低灵敏度的误差的影响，并且需要绝对温度确定的参考。作为替代品，全氟三丁胺（PFTBA）是一种用于19 F MRI测温的全氟化碳液体，基于化学位移响应性，接近1H MRI测温剂的灵敏度;然而，环境持久性、温室气体问题和可能导致MRI伪影的多重共振表明需要替代传感器。利用19 F核磁共振为基础的合成有机氟分子的结构-性质研究，本研究开发了新的有机氟液体，具有改善的温度响应性，高信号，减少非磁性等效氟共振。使用反相HPLC和定量19 F NMR的环境降解分析表明，通过温度传感器的芳基氟核心介导的快速降解曲线。我们的研究结果表明，我们的铅液体温度传感器，DD-1，可以在一个高产量的一个步骤，并具有改进的响应比我们以前的工作和83%的水热响应比PFTBA增加。降解研究表明，在光解条件下，母体化合物会发生强烈降解，半衰期不到两小时，并形成其他氟化产品。DD-1的性能改进及其对环境降解的敏感性突出了一种用于测温应用的新型氟化铅液体。
Accurate temperature measurement via magnetic resonance is valuable for bothin vitroandin vivoanalysis of local tissue for evaluating disease pathology and medical interventions.1H MRI-based thermometry is used clinically but is susceptible to error from magnetic field drift and low sensitivity in fatty tissue and requires a reference for absolute temperature determination. As an alternative, perfluorotributylamine (PFTBA), a perfluorocarbon liquid for19F MRI thermometry, is based on chemical shift responsiveness and approaches the sensitivity of1H MRI thermometry agents; however, environmental persistence, greenhouse gas concerns, and multiple resonances which can lead to MRI artifacts indicate a need for alternative sensors. Using a19F NMR-based structure–property study of synthetic organofluorine molecules, this research develops new organofluorine liquids with improved temperature responsiveness, high signal, and reduced nonmagnetically equivalent fluorine resonances. Environmental degradation analysis using reverse-phase HPLC and quantitative19F NMR demonstrates a rapid degradation profile mediated via the aryl fluorine core of temperature sensors. Our findings show that our lead liquid temperature sensor,DD-1, can be made in high yield in a single step and possesses an improved responsiveness over our prior work and an 83% increase in aqueous thermal responsiveness over PFTBA. Degradation studies indicate robust degradation with half-lives of less than two hours under photolysis conditions for the parent compound and formation of other fluorinated products. The improved performance ofDD-1and its susceptibility to environmental degradation highlight a new lead fluorous liquid for thermometry applications.