Gater Callum A, Mayne Orry J, Collins Benjamin G, Evans Kieren J, Storr Eleanor M E, Whitwood Adrian C, Watts Daniel P, Tickner Ben J, Duckett Simon B
Centre for Hyperpolarization in Magnetic Resonance, University of York, Heslington YO10 5NY, United Kingdom.
Department of Chemistry, University of York, Heslington YO10 5DD, United Kingdom.
J Phys Chem Lett. 2025 Jan 16;16(2):510-517. doi: 10.1021/acs.jpclett.4c03190. Epub 2025 Jan 5.
This research uses perfluorocarbons (PFCs) as effective alternatives to traditional toxic solvents in reversible -hydrogen-induced polarization (PHIP) for NMR signal enhancement. Hydrogen solubility in PFCs is shown here to be an order of magnitude higher than in typical organic solvents by determination of Henry's constants. We demonstrate how this high H solubility enables the PFCs to deliver substantial polarization transfer from -hydrogen, achieving up to 2400-fold signal gains for H NMR detection and 67,000-fold (22% polarization) for N NMR detection at 9.4 T in substrates such as pyridine and nicotine. Notably, methylperfluorobutylether outperforms catalytic efficiency in methanol- and dichloromethane- for pyridine at low catalyst loadings. This makes PFCs particularly advantageous for applications demanding high NMR sensitivity. With high polarization efficiency and reduced toxicity, PFCs hold strong potential for expanding hyperpolarized NMR applications across the biomedical and analytical fields.
本研究使用全氟碳化合物（PFCs）作为传统有毒溶剂的有效替代品，用于可逆氢诱导极化（PHIP）以增强核磁共振（NMR）信号。通过测定亨利常数，结果表明氢气在PFCs中的溶解度比在典型有机溶剂中高一个数量级。我们展示了这种高氢溶解度如何使PFCs能够实现从氢的大量极化转移，在9.4 T磁场下，对于吡啶和尼古丁等底物，氢核磁共振检测的信号增益高达2400倍，氮核磁共振检测的信号增益高达67000倍（22%极化）。值得注意的是，在低催化剂负载量下，甲基全氟丁基醚在吡啶的催化效率方面优于甲醇和二氯甲烷。这使得PFCs对于要求高NMR灵敏度的应用特别有利。凭借高极化效率和降低的毒性，PFCs在扩展生物医学和分析领域的超极化NMR应用方面具有强大的潜力。
