Bondar Oksana A, Moustafa Gamal A I, Robertson Thomas B R
School of Chemistry, Highfield Campus, Southampton, SO17 1BJ, UK.
ATDBio (Now Part of Biotage), Highfield Campus, Southampton, SO17 1BJ, UK.
Analyst. 2024 Nov 18;149(23):5668-5674. doi: 10.1039/d4an01005a.
Signal Amplification By Reversible Exchange (SABRE) can provide strong signal enhancement (SE) to an array of molecules through reversible exchange of parahydrogen (pH) derived hydrides and a suitable substrate coordinated to a transition metal. Among the substrates that can be used as a probe for hyperpolarised NMR and MRI, pyruvate has gained much attention. SABRE can hyperpolarise pyruvate in a low cost, fast, and reversible fashion that does not involve technologically demanding equipment. Most SABRE polarization studies have been done using methanol-d as a solvent, which is not suitable for application. The main goal of this work was to obtain hyperpolarized pyruvate in a solvent other than methanol which may open the door to further purification steps and enable a method to polarize pyruvate in water in future. This work demonstrates hyperpolarization of the [2-C]pyruvate as well as [1-C]pyruvate by SABRE in an acetone/water solvent system at room temperature as an alternative to methanol, which is commonly used. NMR signals are detected using a 1.1 T benchtop NMR spectrometer. In this work we have primarily focused on the study of [2-C]pyruvate and investigated the effect of catalyst concentration, DMSO presence and water acetone solvent concentration on the signal enhancement. The relaxation times for [2-C]-pyruvate solutions are reported in the hope of informing the development of future purification methods.
通过可逆交换实现信号放大（SABRE）可通过对映体氢（pH）衍生的氢化物与配位到过渡金属的合适底物进行可逆交换，为一系列分子提供强信号增强（SE）。在可用作超极化核磁共振（NMR）和磁共振成像（MRI）探针的底物中，丙酮酸备受关注。SABRE能够以低成本、快速且可逆的方式使丙酮酸超极化，且不涉及技术要求高的设备。大多数SABRE极化研究是使用氘代甲醇作为溶剂进行的，这不适合实际应用。这项工作的主要目标是在甲醇以外的溶剂中获得超极化丙酮酸，这可能为进一步的纯化步骤打开大门，并在未来实现一种在水中使丙酮酸极化的方法。这项工作展示了在室温下，通过SABRE在丙酮/水溶剂体系中使[2-C]丙酮酸以及[1-C]丙酮酸超极化，以此替代常用的甲醇。使用1.1 T台式NMR光谱仪检测NMR信号。在这项工作中，我们主要专注于[2-C]丙酮酸的研究，并研究了催化剂浓度、二甲基亚砜（DMSO）的存在以及水 - 丙酮溶剂浓度对信号增强的影响。报告了[2-C]-丙酮酸溶液的弛豫时间，以期为未来纯化方法的开发提供参考。
