Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, 52074 Aachen, Germany.
Department of Chemistry, North Carolina State University, Raleigh, NC 27695, USA.
Int J Mol Sci. 2023 Jan 27;24(3):2465. doi: 10.3390/ijms24032465.
hydrogen (-H)-based techniques are known to drastically enhance NMR signals but are usually limited by -H supply. This work reports -H-based SABRE hyperpolarization at -H pressures of hundreds of bar, far beyond the typical ten bar currently reported in the literature. A recently designed high-pressure setup was utilized to compress -H gas up to 200 bar. The measurements were conducted using a sapphire high-pressure NMR tube and a 43 MHz benchtop NMR spectrometer. In standard methanol solutions, it could be shown that the signal intensities increased with pressure until they eventually reached a plateau. A polarization of about 2%, equal to a molar polarization of 1.2 mmol L, could be achieved for the sample with the highest substrate concentration. While the signal plateaued, the H solubility increased linearly with pressure from 1 to 200 bar, indicating that -H availability is not the limiting factor in signal enhancement beyond a certain pressure, depending on sample composition. Furthermore, the possibility of using liquefied ethane and compressed CO as removable solvents for hyperpolarization was demonstrated. The use of high pressures together with quickly removable organic/non-organic solvents represents an important breakthrough in the field of hyperpolarization, advancing SABRE as a promising tool for materials science, biophysics, and molecular imaging.
基于氢(-H)的技术众所周知可以极大地增强 NMR 信号,但通常受到 -H 供应的限制。本工作报告了 -H 基 SABRE 超极化在数百巴的 -H 压力下的应用,远远超过了文献中目前报道的通常为 10 巴的范围。最近设计的高压装置用于将 -H 气体压缩至 200 巴。使用蓝宝石高压 NMR 管和 43 MHz 台式 NMR 光谱仪进行了测量。在标准甲醇溶液中,可以证明信号强度随压力增加,直到最终达到平台。对于具有最高基质浓度的样品,可以实现约 2%的极化,相当于 1.2 mmol L 的摩尔极化。虽然信号达到平台,但 H 溶解度随压力从 1 到 200 巴线性增加,表明在一定压力以上,-H 的可用性不是信号增强的限制因素,这取决于样品组成。此外,还证明了使用液化乙烷和压缩 CO 作为可去除溶剂进行超极化的可能性。高压与快速可去除有机/无机溶剂的结合代表了超极化领域的重要突破,使 SABRE 成为材料科学、生物物理学和分子成像领域的有前途的工具。